Publications by authors named "Shaojun Dong"

401 Publications

Glucose-oxidase like catalytic mechanism of noble metal nanozymes.

Nat Commun 2021 06 7;12(1):3375. Epub 2021 Jun 7.

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Jilin, PR China.

Au nanoparticles (NPs) have been found to be excellent glucose oxidase mimics, while the catalytic processes have rarely been studied. Here, we reveal that the process of glucose oxidation catalyzed by Au NPs is as the same as that of natural glucose oxidase, namely, a two-step reaction including the dehydrogenation of glucose and the subsequent reduction of O to HO by two electrons. Pt, Pd, Ru, Rh, and Ir NPs can also catalyze the dehydrogenation of glucose, except that O is preferably reduced to HO. By the electron transfer feature of noble metal NPs, we overcame the limitation that HO must be produced in the traditional two-step glucose assay and realize the rapid colorimetric detections of glucose. Inspired by the electron transport pathway in the catalytic process of natural enzymes, noble metal NPs have also been found to mimic various enzymatic electron transfer reactions including cytochrome c, coenzymes as well as nitrobenzene reductions.
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http://dx.doi.org/10.1038/s41467-021-23737-1DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8184917PMC
June 2021

Atomic engineering of single-atom nanozymes for enzyme-like catalysis.

Chem Sci 2020 Aug 11;11(36):9741-9756. Epub 2020 Aug 11.

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences Changchun Jilin 130022 China

Enzyme mimics, especially nanozymes, play a crucial role in replacing natural enzymes for diverse applications related to bioanalysis, therapeutics and other enzyme-like catalysis. Nanozymes are catalytic nanomaterials with enzyme-like properties, which currently face formidable challenges with respect to their intricate structure, properties and mechanism in comparison with enzymes. The latest emergence of single-atom nanozymes (SAzymes) undoubtedly promoted the nanozyme technologies to the atomic level and provided new opportunities to break through their inherent limitations. In this perspective, we discuss key aspects of SAzymes, including the advantages of the single-site structure, and the derived synergetic enhancements of enzyme-like activity, catalytic selectivity and the mechanism, as well as the superiority in biological and catalytic applications, and then highlight challenges that SAzymes face and provide relevant guidelines from our point of view for the rational design and extensive applications of SAzymes, so that SAzyme may achieve its full potential as the next-generation nanozyme.
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http://dx.doi.org/10.1039/d0sc03522jDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8162425PMC
August 2020

FeS nanoparticles decorated carbonized Luffa cylindrica as biofilm substrates for fabricating high performance biosensors.

Talanta 2021 Sep 19;232:122416. Epub 2021 Apr 19.

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, PR China; University of the Chinese Academy of Sciences, Beijing, 100049, PR China. Electronic address:

A high-performance microbial biosensor was fabricated with a reasonably designed biofilm substrate, where the aerogel of carbonized Luffa cylindrica (LC) was used as the scaffold for loading biofilm and FeS nanoparticles (FeSNPs) were employed to modify this aerogel (FeSNPs/Gel). The fabricated FeSNPs/Gel exhibited a spring-like structure similar with that of the raw LC, which facilitated the linkage of the scaffold and promoted its mechanical strength, and further prolonged the service period of the as-prepared biosensor from few days to two months. Meanwhile, the introduced FeSNPs improved the microbial electron transfer of the biofilm and causing an increase in the sensor's signals from 155.0 ± 2.6 to 352.0 ± 17.1 nA and a decrease in the detection limit from 0.95 to 0.38 mg O L (S/N = 3) for the detection of glucose-glutamic acid (GGA). More important, the FeSNPs had been demonstrated to have the capability for modulating a persistent shift of the microbial community with organic pollutant biodegradability. Compared with the Gel, the FeSNPs/Gel exhibited a promising performance for measuring the synthetic sewage and real water samples in BOD assay and an increasing inhibition-ratio for detecting 3,5-dichlorophenol (DCP) in toxicity assay. Based on the vast resource and renewability of LC, this work pave a new avenue for developing high-performance microbial biosensors that are expected to be the engineering production.
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http://dx.doi.org/10.1016/j.talanta.2021.122416DOI Listing
September 2021

Interfacial Electron Engineering of Palladium and Molybdenum Carbide for Highly Efficient Oxygen Reduction.

J Am Chem Soc 2021 May 29;143(18):6933-6941. Epub 2021 Apr 29.

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin 130022, China.

Interfacial electron engineering between noble metal and transition metal carbide is identified as a powerful strategy to improve the intrinsic activity of electrocatalytic oxygen reduction reaction (ORR). However, this short-range effect and the huge structural differences make it a significant challenge to obtain the desired electrocatalyst with atomically thin noble metal layers. Here, we demonstrated the combinatorial strategies to fabricate the heterostructure electrocatalyst of MoC-coupled Pd atomic layers (AL-Pd/MoC) by precise control of metal-organic framework confinement and covalent interaction. Both atomic characterizations and density functional theory calculations uncovered that the strong electron effect imposed on Pd atomic layers has intensively regulated the electronic structures and d-band center and then optimized the reaction kinetics. Remarkably, AL-Pd/MoC showed the highest ORR electrochemical activity and stability, which delivered a mass activity of 2.055 A mg at 0.9 V, which is 22.1, 36.1, and 80.3 times higher than Pt/C, Pd/C, and Pd nanoparticles, respectively. The present work has developed a novel approach for atomically noble metal catalysts and provides new insights into interfacial electron regulation.
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http://dx.doi.org/10.1021/jacs.1c00656DOI Listing
May 2021

CoFe NPs confined in yolk-shell N-doped carbon: engineering multi-beaded fibers as an efficient bifunctional electrocatalyst for Zn-air batteries.

Nanoscale 2021 Jan 25;13(4):2609-2617. Epub 2021 Jan 25.

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China. and University of Science and Technology of China, Hefei 230026, China.

The development of bifunctional catalysts with a delicate structure, high efficiency, and good durability for the oxygen evolution reaction (ORR) and oxygen evolution reaction (OER) is crucial to renewable Zn-air batteries. In this work, CoFe alloy nanoparticles (NPs) confined in N-doped carbon with a yolk-shell structure in multi-beaded fibers were prepared as a bifunctional electrocatalyst. The confinement structure was composed of an N-doped graphitized carbon shell and a core formed by numerous CoFe NPs, and was evenly threaded into a one-dimensional fiber. Moreover, this distinctive hierarchical structure featured abundant mesopores, a high BET surface area of 743.8 m g, good electronic conductivity, and uniformly distributed CoFe/Co(Fe)-N coupling active sites. Therefore, the experimentally optimized [email protected] showed excellent OER performance (overpotential reached 314 mV at 10 mA cm) that far exceeded RuO (353 mV), and good ORR catalytic performance (half-wave potential of 0.827 V) comparable to Pt/C (0.818 V). Impressively, the [email protected] Zn-air battery delivered a higher open circuit voltage of 1.449 V, large power density of 85.7 mW cm, and outstanding charge-discharge cycling stability compared with the commercial RuO + 20 wt% Pt/C catalyst. This work provides new ideas for the structural design of electrocatalysts and energy conversion systems.
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http://dx.doi.org/10.1039/d0nr08781eDOI Listing
January 2021

Low-Noise Solid-State Nanopore Enhancing Direct Label-Free Analysis for Small Dimensional Assemblies Induced by Specific Molecular Binding.

ACS Appl Mater Interfaces 2021 Mar 21;13(8):9482-9490. Epub 2021 Jan 21.

State Key Lab of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin 130022, P. R. China.

Solid-state nanopores show special potential as a new single-molecular characterization for nucleic acid assemblies and molecular machines. However, direct recognition of small dimensional species is still quite difficult due the lower resolution compared with biological pores. We recently reported a very efficient noise-reduction and resolution-enhancement mechanism via introducing high-dielectric additives (e.g., formamide) into conical glass nanopore (CGN) test buffer. Based on this advance, here, for the first time, we apply a bare CGN to directly recognize small dimensional assemblies induced by small molecules. Cocaine and its split aptamer (Capt assembly) are chosen as the model set. By introducing 20% formamide into CGN test buffer, high cocaine-specific distinguishing of the 113 nt Capt assembly has been realized without any covalent label or additional signaling strategies. The signal-to-background discrimination is much enhanced compared with control characterizations such as gel electrophoresis and fluorescence resonance energy transfer (FRET). As a further innovation, we verify that low-noise CGN can also enhance the resolution of small conformational/size changes happening on the side chain of large dimensional substrates. Long duplex concatamers generated from the hybridization chain reaction (HCR) are selected as the model substrates. In the presence of cocaine, low-noise CGN has sensitively captured the current changes when the 26 nt aptamer segment is assembled on the side chain of HCR duplexes. This paper proves that the introduction of the low-noise mechanism has significantly improved the resolution of the solid-state nanopore at smaller and finer scales and thus may direct extensive and deeper research in the field of CGN-based analysis at both single-molecular and statistical levels, such as molecular recognition, assembly characterization, structure identification, information storage, and target index.
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http://dx.doi.org/10.1021/acsami.0c20359DOI Listing
March 2021

A naked-eye readout self-powered electrochemical biosensor toward indoor formaldehyde: On-site detection and exposure risk warning.

Biosens Bioelectron 2021 Apr 6;177:112975. Epub 2021 Jan 6.

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, China; University of Science and Technology of China, Hefei, 230026, China. Electronic address:

The determination of indoor formaldehyde is of great importance to protect individuals against its well-known adverse impact on health. Here, we report on a design of a naked-eye readout self-powered electrochemical biosensor (SPEB) toward gaseous formaldehyde based on the efficient catalytic activity of the formaldehyde dehydrogenase/poly (methylene green)/buckypaper bioanode and the excellent electrochromic property of the Prussian blue (PB) cathode. The SPEB has a planar configuration and is covered with poly(vinyl alcohol) (PVA) as gel electrolyte to provide an inner lateral resistance large enough to enable the progressive discoloration of the patterned PB at cathode, which in turn, making the determination of gaseous formaldehyde feasible by measuring the distance consumed after 10-min exposure. The use of PVA gel electrolyte can also facilitate the observation of the color change due to its excellent transparency. The SPEB shows obvious responses to gaseous formaldehyde in a broad concentration range of 80 and 3000 ppb, covering the important permissible limits of indoor formaldehyde related to human health. The SPEB also exhibits satisfactory results in sensing gaseous formaldehyde released from the real plywood that is one of the dominating sources of the gaseous indoor formaldehyde. The results shown here demonstrate the good potential of the naked-eye readout SPEB as a fast, reliable, and portable tool for on-site determination of gaseous formaldehyde, with the appealing characteristics such as ease of operation, simplicity of configuration, and no requirement of external power sources.
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http://dx.doi.org/10.1016/j.bios.2021.112975DOI Listing
April 2021

Lithium-Ion-Assisted Ultrafast Charging Double-Electrode Smart Windows with Energy Storage and Display Applications.

ACS Cent Sci 2020 Dec 28;6(12):2209-2216. Epub 2020 Oct 28.

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin 130022, China.

Lithium-ion-assisted ultrafast charging double-electrode smart windows with energy storage and a fluorescence display device (FTO/PB/[email protected]||[email protected]/WO/FTO) based on double electrochromic electrodes (cathode and anode) (FSDECEs) have been designed and fabricated. Here, Prussian blue (PB) and WO are selected as the electrochromic cathode and anode, respectively. There is a synergistic effect and a large potential difference between the two electrodes. They could be simultaneously and rapidly bleached after being connected with each other. Also, the fluorescence intensity of [email protected] nanoparticles (NPs) could be regulated by the fluorescence resonance energy transfer effect (FRET). After discharging, the two electrochromic electrodes in the bleached state can be recharged by a Mg-O battery with a FeN single atomic catalyst to quickly recover the colored state. The double electrochromic electrodes can reversibly alter between coloring and bleaching states only by connecting and disconnecting the electrodes. The fluorescence intensity of FSDECEs can switch between quenching and emission, thus endowing the "on" and "off" functions. The system is concise, environmentally friendly, and easy to operate. The proposed FSDECEs demonstrate high fluorescence contrast, a fast response time, and long-term stability. Such an ingenious design of fluorescence switching based on the double electrochromic electrode in a single cell sheds light on next-generation transparent, portable, and self-powered electrochromic devices and electronic equipment.
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http://dx.doi.org/10.1021/acscentsci.0c01149DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7760464PMC
December 2020

Propelling DNA Computing with Materials' Power: Recent Advancements in Innovative DNA Logic Computing Systems and Smart Bio-Applications.

Adv Sci (Weinh) 2020 Dec 9;7(24):2001766. Epub 2020 Nov 9.

State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences Changchun Jilin 130022 China.

DNA computing is recognized as one of the most outstanding candidates of next-generation molecular computers that perform Boolean logic using DNAs as basic elements. Benefiting from DNAs' inherent merits of low-cost, easy-synthesis, excellent biocompatibility, and high programmability, DNA computing has evoked substantial interests and gained burgeoning advancements in recent decades, and also exhibited amazing magic in smart bio-applications. In this review, recent achievements of DNA logic computing systems using multifarious materials as building blocks are summarized. Initially, the operating principles and functions of different logic devices (common logic gates, advanced arithmetic and non-arithmetic logic devices, versatile logic library, etc.) are elaborated. Afterward, state-of-the-art DNA computing systems based on diverse "toolbox" materials, including typical functional DNA motifs (aptamer, metal-ion dependent DNAzyme, G-quadruplex, i-motif, triplex, etc.), DNA tool-enzymes, non-DNA biomaterials (natural enzyme, protein, antibody), nanomaterials (AuNPs, magnetic beads, graphene oxide, polydopamine nanoparticles, carbon nanotubes, DNA-templated nanoclusters, upconversion nanoparticles, quantum dots, etc.) or polymers, 2D/3D DNA nanostructures (circular/interlocked DNA, DNA tetrahedron/polyhedron, DNA origami, etc.) are reviewed. The smart bio-applications of DNA computing to the fields of intelligent analysis/diagnosis, cell imaging/therapy, amongst others, are further outlined. More importantly, current "Achilles' heels" and challenges are discussed, and future promising directions of this field are also recommended.
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http://dx.doi.org/10.1002/advs.202001766DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7740092PMC
December 2020

Fabrication of a Novel, Cost-Effective Double-Sided Indium Tin Oxide-Based Nanoribbon Electrode and Its Application of Acute Toxicity Detection in Water.

ACS Sens 2020 12 11;5(12):3923-3929. Epub 2020 Dec 11.

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Science, Changchun, Jilin 130022, P. R. China.

Microelectrode plays a crucial role in developing a rapid biosensor for detecting toxicity in water. In this study, a nanoribbon electrode (NRE) with amplified microelectrode signal was successfully prepared by electrodepositing 2-allylphenol on a double-sided indium tin oxide glass. The NRE provided a simple mean for obtaining large steady-state current response. Its advantages were discussed by contrasting the toxicity detection of 3,5-dichlorophenol (DCP) with single microelectrode, microelectrode array, and millimeter electrode as working electrodes in which potassium ferricyanide (K[Fe(CN)]) was adopted as a mediator, and was selected as bioreceptor. At a constant potential of 450 mV, the current reached a steady state within 10 s. The biosensor was constructed using the NRE as working electrode, and its feasibility was verified by determining the toxicity of DCP. A 50% inhibitory concentration (IC) of 3.01 mg/L was obtained by analyzing the current responses of different concentrations of DCP within 1 h. These results exhibited that the proposed method based on the as-prepared NRE was a rapid, sensitive, and cost-effective way for toxicity detection in water.
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http://dx.doi.org/10.1021/acssensors.0c01566DOI Listing
December 2020

Coenzyme-dependent nanozymes playing dual roles in oxidase and reductase mimics with enhanced electron transport.

Nanoscale 2020 Dec;12(46):23578-23585

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin 130022, PR China.

Although nanozymes overcome a series of shortcomings of natural enzymes, their wide applications are hampered due to their limited varieties. In this work, we propose a coenzyme-dependent nanozyme, a synergistic composite comprising zeolitic imidazolate frameworks encapsulated with polyethylenimine (PEI) and functionalized with a flavin mononucleotide (PEI/ZIF-FMN). The flavin mononucleotide (FMN) plays the role of a prosthetic group, and the positively charged NH2 groups in PEI readily provide the binding affinity to nicotinamide adenine dinucleotide (NADH), which facilitates the electron transfer from NADH to FMN and terminal electron acceptors (such as O2) with a greatly enhanced (80 times) catalytic performance. The integrated nanoparticle-coenzyme composite works as an NADH oxidase mimic and couples with dehydrogenases for the tandem enzymatic reaction. PEI/ZIF-FMN also mediated the electron transfer from NADH to cytochrome c (Cyt c), thereby exhibiting Cyt c reductase-like activity.
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http://dx.doi.org/10.1039/d0nr06605bDOI Listing
December 2020

A comparison study of test organism species and methodologies for combined toxicity assay of copper ions and zinc ions.

Environ Sci Pollut Res Int 2020 Dec 2;27(36):45992-46002. Epub 2020 Nov 2.

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, People's Republic of China.

The general toxicity assays for evaluating the risk of aquatic environment were commonly based on single-species test organism models. Thus, the lack and conflict of the different responses among species had hindered researchers to assess the real toxicity of a target toxicant. Therefore, the difference between the test species and their corresponding methodologies was investigated in this work and three species, Escherichia coli, Saccharomyces cerevisiae and Misgurnus anguillicaudatus (a fish), were chosen as the test organism for typical prokaryotes, eukaryotes, and vertebrates, respectively. More specifically, we investigated (i) the individual and combined toxicity of Cu and Zn by the three test organisms; (ii) the different evaluation manners for the test organisms, including IC and toxic unit (TU) model for microorganisms by respiratory toxicity assay and enzyme-substrate assay, while survival time for fish; and (iii) the states of test organism, including suspended and immobilized states for microorganisms. The combined effects, including synergistic (Vt < Vp), antagonistic (Vt > Vp) and additive effects for the three species, were complex as that they were usually dose-dependent and could be changed by the different evaluation manners. The present work was useful for enriching of the associated theory and the insights from this work could open the way for further practical risk assessments.
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http://dx.doi.org/10.1007/s11356-020-11444-1DOI Listing
December 2020

Synthesis of low dimensional hierarchical transition metal oxides a direct deep eutectic solvent calcining method for enhanced oxygen evolution catalysis.

Nanoscale 2020 Oct;12(40):20719-20725

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin 130022, P. R. China. and University of Science and Technology of China, Hefei, Anhui 230026, P. R. China and University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.

Transition metal oxides (TMOs) are regarded as important materials due to their wide applications in catalysis, sensors, energy storage and conversion devices owing to their advantages of facile synthesis, low cost, and high activity. Here we develop a direct deep eutectic solvent (DES) calcining method to prepare low-dimensional and highly active TMOs for the electrochemical oxygen evolution reaction (OER). Glucose monohydrate and urea can form a glucose-urea DES, which was calcined under a N2 atmosphere to produce 2D N,O-doped graphene. When metal precursors were introduced into the glucose-urea DES and calcined together, the TMOs were templated by graphene flakes and exhibited low-dimensional morphologies. With this method, 2D nanonet-shaped La0.5Sr0.5Co0.8Fe0.2O3 (LSCF), Co3O4, NiCo2O4, and RuO2 and 1D nanowire-shaped Ba0.5Sr0.5Co0.8Fe0.2O3 (BSCF) were readily synthesized, and their thickness and porosity can be conveniently tuned by adjusting the concentrations of metal salts. Our nanostructured TMOs were further applied for the OER, and they showed quite competitive activities over their counterparts obtained from other methods. The 2D porous LSCF20-DES exhibited the largest specific surface area (28.9 m2 g-1) and the highest OER electrocatalytic activities (0.304 V overpotential at a current density of 10 mA cm-2). These results demonstrate that the DES calcining method is a comprehensive approach to synthesize hierarchical TMOs as highly active OER catalysts.
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http://dx.doi.org/10.1039/d0nr04378hDOI Listing
October 2020

Oxidase-like MOF-818 Nanozyme with High Specificity for Catalysis of Catechol Oxidation.

J Am Chem Soc 2020 09 27;142(36):15569-15574. Epub 2020 Aug 27.

College of Chemistry, Jilin University, Changchun 130012, P. R. China.

Despite the extensive studies of the nanozymes showing their superior properties compared to natural enzymes and traditional artificial enzymes, the development of highly specific nanozymes is still a challenge. The catechol oxidase specifically catalyzing the oxidations of -diphenol to the corresponding -quinone is important to the biosynthesis of melanin and other polyphenolic natural products. In this study, we first propose that MOF-818, containing trinuclear copper centers mimicking the active sites of natural catechol oxidase, shows efficient catechol oxidase activity with good specificity and no peroxidase-like characteristics. MOF-818 has good specificity and high catalytic activity as a novel catechol oxidase nanozyme.
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http://dx.doi.org/10.1021/jacs.0c07273DOI Listing
September 2020

An unexpected discovery of 1,4-benzoquinone as a lipophilic mediator for toxicity detection in water.

Analyst 2020 Aug 10;145(15):5266-5272. Epub 2020 Jul 10.

Key Laboratory of Wetland Ecology and Environment, Northeast Institute of Geography and Agroecology, Chinese Academy of Science, Changchun 130102, Jilin, P. R. China.

Since most toxicological risk assessments are based on individual single-species tests, there is uncertainty in extrapolating these results to ecosystem assessments. Herein, we successfully developed a mediated microbial electrochemical biosensor with mixed microorganisms for toxicity detection by microelectrode array (MEA). In order to fully mobilize all the mixed microorganisms to participate in electron transfer to amplify the current signal, 1,4-benzoquinone (BQ) was used as the lipophilic mediator to mediate the intracellular metabolic activities. Hydrophilic K[Fe(CN)] was employed as an extracellular electron acceptor to transport electrons from hydroquinone (HQ) to the working electrode. Under the optimal conditions of 50 mM phosphate buffer solution (PBS), 0.4 mM BQ, 10 mM K[Fe(CN)] and OD = 0.5 bacteria concentration, the half-maximal inhibitory concentration (IC) values measured with the composite-mediated respiration (CM-RES) of BQ-K[Fe(CN)] for Cu, Cd and Zn were 5.95, 7.12 and 8.86 mg L, respectively. IC values obtained with the single mediator K[Fe(CN)] were 2.34, 5.88 and 2.42 mg L for the same samples. The results indicate that the biosensor with the single mediator K[Fe(CN)] had higher sensitivity to heavy metal ions than the biosensor with composite mediators. After verification, we found that the addition of BQ cannot amplify the current. The IC value of 0.89 mg L for BQ was obtained using K[Fe(CN)] as the single mediator. This suggests that BQ is highly toxic, which explained why the sensitivity of the biosensor with the combined mediator BQ-K[Fe(CN)] was lower than that of the biosensor with the single mediator K[Fe(CN)]. At the same time, this also implies that toxicity itself cannot be ignored when it is used as an electronic mediator in a mediated microbial electrochemical biosensor.
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http://dx.doi.org/10.1039/d0an00991aDOI Listing
August 2020

Recent development of biofuel cell based self-powered biosensors.

J Mater Chem B 2020 04;8(16):3393-3407

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China.

Self-powered biosensors (SPBs) based on enzymatic biofuel cells (EFCs) and microbial fuel cells (MFCs) have attracted considerable attention due to their obvious advantages such as simple configuration and ease of miniaturization, and potential applications including clinical diagnosis, environmental monitoring, industrial process control, etc. In this review, we will summarize the recent advances in SPBs, focusing on the use of EFC-SPBs as power sources in combination with microelectronic and electrochromic devices, and the applications of MFC-based SPBs as sensors for detecting toxicity, chemical oxygen demand (COD), biochemical oxygen demand (BOD) and assimilable organic carbon (AOC). The efforts in, for example, boosting the energy, reducing the cost, and improving the sensing performance in terms of sensitivity, accuracy and dynamic detection range are discussed. Finally, future prospects for the development of MFC-based SPBs are presented.
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http://dx.doi.org/10.1039/c9tb02428jDOI Listing
April 2020

Investigation on the stress response of microbes in acute toxicity assay.

Anal Chim Acta 2020 Feb 18;1099:46-51. Epub 2019 Nov 18.

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, China. Electronic address:

Acute toxicity assay by using microbes as bioindicators is an effective tool for reflecting the impact of water pollution on organisms. Until now, the suspended state of microbes is still mainly adopted, because the immobilized state of microbes will cause the poor stability of toxicity assay due to the microbes being reused. Here, an electrochemical biosensor based on biofilm was established for toxicity assay (TOX-biosensor), and the stress response of immobilized microbes in biofilm was demonstrated as the main factor that resulting in instability of the TOX-biosensor, and it can be induced by both of dose and time accumulation. The intensity of stress response for measuring a toxicant absence of organic substance was triple of that presence, indicating extracellular substances can be used for microbial repair and result in the decrease of the consumption of endogenous substance. Herein, a weak magnetic field (WMF) was employed to balance the activity of biofilm in the present TOX-biosensor, and a low intensity of WMF 10 GS was demonstrated to have the function for weakening stress response. Under this condition, the signals of biosensor can be kept stable for a month and the recovery time of dormant TOX-biosensor can be shorted from 50 h to 10 h. Its mechanism may be associated with the special magnetic field inside the organisms and the charge transfer happened in the life activity process.
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http://dx.doi.org/10.1016/j.aca.2019.11.036DOI Listing
February 2020

Graphitic Carbon Nitride (g-CN)-Derived Bamboo-Like Carbon Nanotubes/Co Nanoparticles Hybrids for Highly Efficient Electrocatalytic Oxygen Reduction.

ACS Appl Mater Interfaces 2020 Jan 16;12(4):4463-4472. Epub 2020 Jan 16.

State Key Laboratory of Electroanalytical Chemistry , Changchun Institute of Applied Chemistry, Chinese Academy of Sciences , Changchun , Jilin 130022 , China.

The oxygen reduction reaction (ORR) is an extremely important reaction in many renewable energy-related devices. The sluggish kinetics of the ORR limits the development of many fuel cells. Design and synthesis of highly efficient nonprecious electrocatalysts are of vital importance for electrochemical reduction of oxygen. Herein, we develop a graphitic carbon nitride (g-CN)-derived bamboo-like carbon nanotubes/carbon-wrapped Co nanoparticles (BCNT/Co) electrocatalyst by a simple high-temperature pyrolysis and acid-leaching method. The catalytic performance of the as-designed electrocatalyst toward ORR outperforms the commercial Pt/C catalyst in alkaline solution. The onset potential of nonprecious BCNT/Co-800 catalyst was 1.12 V. The half-wave potential was 0.881 V. The result was superior to that of commercial Pt/C (0.827 V vs RHE). The Co nanoparticles, bamboo-like carbon nanotubes, defects, and Co-N active sites all result in the remarkable ORR activity, stability, and great methanol tolerance.
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http://dx.doi.org/10.1021/acsami.9b18454DOI Listing
January 2020

Coupling Cu with Au for enhanced electrocatalytic activity of nitrogen reduction reaction.

Nanoscale 2020 Jan;12(3):1811-1816

College of Chemistry, Jilin University, Changchun, Jilin 130012, P.R. China.

The electrochemical nitrogen reduction reaction (NRR) under ambient conditions is currently attracting intense attention, but it still remains a great challenge to develop highly selective and active NRR electrocatalysts. Inspired by the intrinsic NRR activity of Au, we systematically studied the synergistic enhanced effect of incorporating other transition metals into Au on its NRR activity. A general strategy was used to synthesize a series of Au-based bimetallic nanocatalysts (AuCu, AuAg, AuPd and AuRu), and the NRR catalytic performance of the as-obtained electrocatalysts was investigated in detail. The experimental results indicate that the positive effect of Cu on NRR was the most remarkable in comparison with that of Ag, Ru and Pd, which can be ascribed to the synergy of the Au and Cu components via modulating the electronic structure and further changing the binding affinity of adsorbed N atoms on the catalyst. Finally, the optimized nanocatalyst with the atom ratio of Au1Cu1 achieved the highest faradaic efficiency (54.96%) and ammonia yield rate (154.91 μg h-1 mgcat-1) at -0.2 V vs. RHE, exceeding those of the previously reported Au nanocatalysts.
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http://dx.doi.org/10.1039/c9nr08788eDOI Listing
January 2020

How to Identify the "LIVE/DEAD" States of Microbes Related to Biosensing.

ACS Sens 2020 01 8;5(1):258-264. Epub 2020 Jan 8.

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry , Chinese Academy of Sciences , Changchun 130022 , PR China.

In this work, we fabricated a microbial biosensor with long-term stability, which relied on microbial activity. Activity of the microbe was commonly estimated by LIVE/DEAD assay and the propidium iodide (PI)-stained one was judged as dead. Herein, we proposed the utilization of a physiological state of microbes, which was neither live nor dead but between them. In this state, microbes represented a high PI-stained ratio but still had catalytic ability. This microbial state was obtained by forming the biofilm under the conditions of poor nutrition and low temperature. Thus, the dividing and proliferating ability of the microbes in the biofilm was weak, which was beneficial for long-term stability. This mechanism was further confirmed by the biosensors made from multifarious substrate materials, including graphene-based gel, biomass-based gel, graphite felt, and poly(vinyl chloride). This biosensor was applied to water pollution monitoring in the laboratory for 2 years and then was integrated into a multiparameter water quality monitoring station on a local lake for 2.5 years.
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http://dx.doi.org/10.1021/acssensors.9b02138DOI Listing
January 2020

A respiration substrate-less isolation method for acute toxicity assessment.

Chemosphere 2020 Apr 29;244:125511. Epub 2019 Nov 29.

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, PR China. Electronic address:

Respiration substrate (RS)-less isolation method was developed for enhancing the sensitivity of acute toxicity assessment of heavy metal ions. RS was removed from the first step of previous isolation method, which was an effective strategy for improving acute toxicity assessment. 50% inhibiting concentration (IC) values of Cu, Cd, Zn, Hg and Ni were 0.39 mg L, 5.99 mg L, 3.99 mg L, 0.23 mg L and 5.74 mg L, respectively. Beyond that, the complicacy of organic toxicants assessments was investigated by choosing 3,5-dichlorophenol (DCP) as model toxicant. Biofilm sensor, morphology method and suspended microbes-based methods including one-pot method, RS-isolation method, RS-less isolation method, RS-less isolation method with added potassium ferricyanide (+F), were compared. The sensitivity to DCP can be ranked as morphology method > suspended microbes-based methods > biofilm method. The difference of the present results implicated that the methodological interference, leading in different detection mechanisms of these methods. The relative investigations can provide theoretical guidance for developing comprehensive detection methods of pollutants.
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http://dx.doi.org/10.1016/j.chemosphere.2019.125511DOI Listing
April 2020

Fe/N-doped hollow porous carbon spheres for oxygen reduction reaction.

Nanotechnology 2020 Mar 25;31(12):125404. Epub 2019 Nov 25.

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, People's Republic of China. University of Science and Technology of China, Hefei 230026, People's Republic of China.

Herein, we design a dual-template-assisted pyrolysis method to prepare ultra-small FeO nanoparticles anchored on Fe/N-doped hollow porous carbon spheres (0.010-Fe/NHPCS-800) for oxygen reduction reaction (ORR). The synthesized SiO nanospheres, which are selected as the hard template, contribute to forming macroporous structure. Pluronic ® F127 is employed to fabricate mesopores through high-temperature pyrolysis as a soft template. In this way, the 0.010-Fe/NHPCS-800 architecture represents an ordered hierarchically porous property with a large BET surface area (1812 m g), which can facilitate the mass transport of reactants and increase the electrochemically active area. The FeO nanoparticles wrapped by graphitic carbon layers provide more active sites, and the synergistic interaction between FeO nanoparticles and doping N has a positive effect on ORR performance. The 0.010-Fe/NHPCS-800 catalyst outperforms the most effective ORR activities among a series of Fe/NHPCS samples with onset potential of 0.95 V (versus reversible hydrogen potential) and half-wave potential of 0.81 V, which is almost the same as the commercial Pt/C (0.96 and 0.81 V, correspondingly) in 0.10 M KOH. However, both the stability and durability of 0.010-Fe/NHPCS-800 surpass those of commercial Pt/C. Given all these advantages, 0.010-Fe/NHPCS-800 is a promising candidate to take the place of Pt-based electrocatalysts for ORR in the future.
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http://dx.doi.org/10.1088/1361-6528/ab5b56DOI Listing
March 2020

Hydrothermal synthesis of polydopamine-functionalized cobalt-doped lanthanum nickelate perovskite nanorods for efficient water oxidation in alkaline solution.

Nanoscale 2019 Nov 17;11(41):19579-19585. Epub 2019 Oct 17.

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin 130022, China.

Perovskite oxides have attracted great attention recently for their low cost and high intrinsic activity in the electrochemical oxygen evolution reaction (OER). In this work, we synthesized highly efficient OER electrocatalysts in alkaline solution by carbonization of polydopamine (PDA)-functionalized cobalt-doped lanthanum nickelate perovskite nanorod (LaNiCo) complexes. The calcination temperature and molar ratio for La, Ni, and Co were optimized. The as-prepared complex with a molar ratio of 5 : 3 : 2 (La : Ni : Co) and a calcination temperature of 500 °C displayed enhanced OER activity and excellent durability. In 1.0 M KOH, the overpotential of the as-prepared catalyst at a current density of 10 mA cm was 0.360 V, which is comparable to those of noble metal-based materials or perovskite-based materials. The Tafel slope is 48.1 mV dec, which is smaller than those of prepared composites. The satisfactory oxygen evolution activity could be attributed to the increased CoO, O/O, pyridine N, and quaternary N species after calcination treatment, and the improved amount of Ni during the OER process, as well as the high surface area and electrochemical surface area.
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http://dx.doi.org/10.1039/c9nr06519aDOI Listing
November 2019

A Janus-inspired amphichromatic system that kills two birds with one stone for operating a "DNA Janus Logic Pair" (DJLP) library.

Chem Sci 2019 Aug 13;10(30):7290-7298. Epub 2019 Jun 13.

State Key Laboratory of Electroanalytical Chemistry , Changchun Institute of Applied Chemistry , Chinese Academy of Sciences , Changchun , Jilin 130022 , China . Email: ; Email:

Although DNA computing has exhibited a magical power across diverse areas, current DNA logic gates with different functions are always separately operated and can only produce hard-to-visualize output. The fussy/obligatory gates' redesign/reconstruction and the non-intuitive output cause the wastage of time and costs, low efficiency and practicality. Herein, inspired by the ancient Roman mythical God Janus, for the first time, we propose the concept of "DNA Janus Logic Pair" (DJLP) to classify the DNA logic gates with contrary functions into "Positive + Negative" gates (DJLP = Pos + Neg). Based on the biocatalytic property of G-quadruplex DNAzyme (G4zyme) and the luminescence quenching ability of oxidized 3,3',5,5'-tetramethylbenzidine (OxTMB) towards the upconversion (UC) particles, we fabricated a universal amphichromatic platform that kills two birds with one stone for operating a versatile DJLP library. Different from the previous DNA logic systems, the "Pos + Neg" gates of each DJLP in this study were concomitantly achieved the same one-time DNA reaction, which avoided the gates' redesign/reoperation and reduced the operating costs/time of the DNA gates by at least half. Besides, both the amphichromatic outputs (Visual-blue and UC luminescent-green) can be visualized under harmless-NIR, thus bringing greatly enhanced practicality to the method. Moreover, we constructed various concatenated logic circuits logically modulating the G4zyme's biocatalytic property with glutathione, thus enabling the largely improved computing complexity. Furthermore, taking the circuit "YES-INH-1-2 decoder" as the "computing core", we designed an "antioxidant indicator" with ratiometric logical responses that could recognize the presence of antioxidants smartly (output changed from "10" to "01"), which provided a typical prototype for potential intelligent bio-applications.
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http://dx.doi.org/10.1039/c9sc01865dDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6686727PMC
August 2019

Water/Oxygen Circulation-Based Biophotoelectrochemical System for Solar Energy Storage and Release.

J Am Chem Soc 2019 Oct 7;141(41):16416-16421. Epub 2019 Oct 7.

State Key Laboratory of Electroanalytical Chemistry , Changchun Institute of Applied Chemistry, Chinese Academy of Sciences , Changchun , Jilin 130022 , People's Republic of China.

Fabricating an artificial photoelectrochemical device to provide electric power on demand is highly desirable but remains a challenge. In response to the intermittent nature of sunlight, we develop a water/oxygen circulation-based biophotoelectrochemical system (BPECS) by integrating a polypyrrole (PPy) capacitor electrode into a photobiofuel cell (PBFC). Unlike traditional PEC devices, the modular and integrated system design of BPECS can not only improve compatibility among PEC cells, BFCs, and capacitor devices, but also offers a feasible way for tackling the intermittent nature of sunlight. In this system, the molecules of water and oxygen can form a self-circulation, thus making this device intrinsically safe and cost-effective. Through the alternate two-step energy conversion (i.e., solar-to-chemical/electric and chemical-to-electric), this conceptual model obtains maximum power output densities of 0.34 ± 0.01 and 0.19 ± 0.02 mW cm in light and dark conditions, respectively, and presents stable long-term cycling performance for solar energy storage and release. Our results demonstrate that such a BPECS achieves high-effective solar energy utilization, which carries great significance to the development of artificial BPECS and provides research opportunities to explore a deployable route for grid-scale photovoltaic energy storage.
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http://dx.doi.org/10.1021/jacs.9b08046DOI Listing
October 2019

Reversible self-powered fluorescent electrochromic windows driven by perovskite solar cells.

Chem Commun (Camb) 2019 Oct;55(80):12060-12063

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin 130022, China and University of Science and Technology of China, Hefei, Anhui 230026, China and University of Chinese Academy of Sciences, Beijing, 100039, China.

Self-powered electrofluorochromic devices (EFCDs) have attracted particular attention for smart windows of green buildings. In this work, we report a perovskite solar cell (PSC) driven self-powered EFCD. For the first time, electrochromic material polyoxometalates (POMs) and a fluorescent component are made into wet adhesives. A special design feature is that POMs and magnesium composed a battery powering the EFCD bleaching, and the device can be quickly coloured after connecting with the PSCs by the electrical power generated through solar energy conversion. Therefore, without any additional external bias, the fabricated EFCD undergoes an electrochromic transition from white semitransparent to dark blue-tinted, and under UV it presents reversible fluorescence switching between yellow and dark.
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http://dx.doi.org/10.1039/c9cc05779jDOI Listing
October 2019

A Self-Powered Biosensor with a Flake Electrochromic Display for Electrochemical and Colorimetric Formaldehyde Detection.

ACS Sens 2019 10 18;4(10):2631-2637. Epub 2019 Sep 18.

State Key Laboratory of Electroanalytical Chemistry , Changchun Institute of Applied Chemistry, Chinese Academy of Sciences , Changchun 130022 , China.

The formaldehyde biosensors with the features of cost effectiveness, high specificity, easy operation, and simplicity are urgently desired in routing and field detection of formaldehyde. Here, we report a new design of an enzymatic self-powered biosensor (ESPB) toward formaldehyde detection. The ESPB involves a formaldehyde dehydrogenase/poly-methylene green/buckypaper bioanode as the sensing electrode and a Prussian blue/Au nanoparticles/carbon fiber paper cathode as the electrochromic display. Formaldehyde acts as the fuel to drive the ESPB, relying on that the concentration of formaldehyde can be determined with the ESPB by both directly measuring the variance in short circuit current and observing the color change of the cathode. By measuring the variance in short circuit current, a linear detection range from 0.01 to 0.35 mM and a calculated detection limit of 0.006 mM are obtained, comparable to or better than those reported before. The color change of the cathode can be distinguished easily and exactly via the naked eye after immersing the ESPB in formaldehyde solution for 90 s with the concentration up to 0.35 mM, covering the permissive level of formaldehyde in some standards associated with environmental quality control. Specially, the formaldehyde concentration can be precisely quantified by analyzing the color change of the cathode digitally using the equation of /( + + ). In the following test of real spiked samples of tap water and lake water, the recovery ratios of formaldehyde with the concentrations from 0.010 to 0.045 mM are tested to be between 95 and 100% by both measuring the variance in short circuit current and analyzing the color change of the cathode digitally. In addition, the ESPB exhibits negligible interference from acetaldehyde and ethanol and can be stored at 4 °C for 21 days with a loss of less than 8% in its initial value of short circuit current. Therefore, the ESPB with the capability of working like disposable test paper can be expected as a sensitive, simple, rapid, cost-effective colorimetric method with high selectivity in routing and field formaldehyde detection.
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http://dx.doi.org/10.1021/acssensors.9b00917DOI Listing
October 2019

Cobalt doped β-molybdenum carbide nanoparticles encapsulated within nitrogen-doped carbon for oxygen evolution.

Chem Commun (Camb) 2019 Aug;55(67):9995-9998

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Science, Changchun, Jilin 130022, P. R. China.

Herein, we report a novel cobalt doped transition metal carbide-based OER electrocatalyst, cobalt doped β-molybdenum carbide (β-Mo2C) encapsulated by a nitrogen doped carbon framework, Co0.1-β[email protected], which shows an unexpected onset overpotential of 200 mV and an overpotential of 262.2 mV at a current density of 10 mA cm-2. This strategy of cobalt doping reduces the amount of cobalt, and increases the density of active sites as well; furthermore, the introduction of molybdenum carbide enhances the stability of the catalyst.
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http://dx.doi.org/10.1039/c9cc04892hDOI Listing
August 2019

Self-Indicative Gold Nanozyme for H O and Glucose Sensing.

Chemistry 2019 Sep 14;25(51):11940-11944. Epub 2019 Aug 14.

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin, 130022, P.R. China.

In addition to superior enzyme-mimicking abilities, nanozymes also have intrinsic physicochemical properties. Integrating the enzyme-like activities and tunable physicochemical properties into a single nanoparticle is a promising strategy for versatile nanozyme design and application. Herein, a composite nanozyme in which Au nanoparticles are encapsulated by Au nanoclusters ([email protected]) is presented. By integrating the peroxidase-mimicking ability of fluorescent Au NCs with the glucose oxidase-like activity of Au NPs, the composite nanozyme realized cascade assay of glucose without the aid of external indicators. Compared to traditional multistep colorimetric methods, the analytical process was highly simplified by using the self-responsive nanozyme. This synthetic strategy provided valuable insights into exploring talented nanozymes for sensing diverse targets.
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http://dx.doi.org/10.1002/chem.201902288DOI Listing
September 2019

Self-Rechargeable-Battery-Driven Device for Simultaneous Electrochromic Windows, ROS Biosensing, and Energy Storage.

ACS Appl Mater Interfaces 2019 Aug 26;11(31):28072-28077. Epub 2019 Jul 26.

State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry , Chinese Academy of Sciences , Changchun , Jilin 130022 , China.

A self-powered electrochromic device (ECD) powered by a self-rechargeable battery is easily fabricated to achieve electrochromic window design, quantitative reactive oxygen species (ROS) sensing, and energy storage. The special design of the battery was composed of Prussian blue (PB) and magnesium metal as the cathode and anode, respectively, which exhibits fast self-charging and high power-density output for continuous and stable energy supply. Benefitting from the fast electrochromic response of PB, it was not only used for structuring self-rechargeable batteries but also used as an electrochromic display for highly sensitive self-powered ROS sensing and visual analysis. We believe that this work provides a solution to self-powered ECDs limited to a single application and could combine the applications in smart windows, ROS sensing, and other fields together, and in the meantime provide a solution for energy supply problems.
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http://dx.doi.org/10.1021/acsami.9b08715DOI Listing
August 2019