Publications by authors named "Fuyi Wang"

110 Publications

Bottom-Up-Etching Mediated Synthesis of Large-Scale Pure Monolayer Graphene on Cyclic-Polishing-Annealed Cu(111).

Adv Mater 2021 Nov 25:e2108608. Epub 2021 Nov 25.

Beijing National Laboratory for Molecular Sciences, Key Laboratory of Organic Solids, Institute of Chemistry, Beijing, 100190, P. R. China.

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http://dx.doi.org/10.1002/adma.202108608DOI Listing
November 2021

Cooperative Shielding of Bi-Electrodes via In Situ Amorphous Electrode-Electrolyte Interphases for Practical High-Energy Lithium-Metal Batteries.

J Am Chem Soc 2021 Oct 4;143(40):16768-16776. Epub 2021 Oct 4.

CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Center for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences (CAS), Beijing 100190, P. R. China.

Solid-state Li-metal batteries offer a great opportunity for high-security and high-energy-density energy storage systems. However, redundant interfacial modification layers, intended to lead to an overall satisfactory interfacial stability, dramatically debase the actual energy density. Herein, a dual-interface amorphous cathode electrolyte interphase/solid electrolyte interphase CEI/SEI protection (DACP) strategy is proposed to conquer the main challenges of electrochemical side reactions and Li dendrites in hybrid solid-liquid batteries without sacrificing energy density via LiDFOB and LiBF in situ synergistic conversion. The amorphous CEI/SEI products have an ultralow mass proportion and act as a dynamic shield to cooperatively enforce dual electrodes with a well-preserved structure. Thus, this in situ DACP layer subtly reconciles multiple interfacial compatibilities and a high energy density, endowing the hybrid solid-liquid Li-metal battery with a sustainably brilliant cycling stability even at practical conditions, including high cathode loading, high voltage (4.5 V), and high temperature (45 °C) conditions, and enables a high-energy-density (456 Wh kg) pouch cell (11.2 Ah, 5 mA h cm) with a lean electrolyte (0.92 g Ah, containing solid and liquid phases). The compatible modification strategy points out a promising approach for the design of practical interfaces in future solid-state battery systems.
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http://dx.doi.org/10.1021/jacs.1c08425DOI Listing
October 2021

High Voltage-Stabilized Graphdiyne Cathode Interface.

Small 2021 Sep 8;17(38):e2102066. Epub 2021 Aug 8.

Beijing National Laboratory for Molecular Sciences (BNLMS), CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry, Chinese Academy of Science, Beijing, 100190, P. R. China.

Suppressing the irreversible interfacial reactions is an important scientific bottleneck in the development of stable high-energy-density lithium-ion battery. The interfacial chemistry of graphdiyne (GDY) on the high-voltage cathode of LiNi Mn O (LNMO) shows a very interesting process, in which the sp-hybridization carbon atoms chemically scavenge the hydrofluoric acid (HF) and in situ form the fluorinated GDY interface. It first turns the harmful HF into profit, and greatly enhances the interfacial stability and restrains the side reaction on the cathode under high working voltage. The GDY-coated LNMO cathode obviously alleviates the electrolyte degradation, achieves high Coulombic efficiency and reliability. Due to atomic-level selectivity and chemical trapping of HF by GDY, it effectively suppresses the dissolution of Mn, Ni elements. These results highlight the unparalleled advantages of GDY in the formation of high stable interfaces and protection of high-energy-density electrodes.
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http://dx.doi.org/10.1002/smll.202102066DOI Listing
September 2021

A Facile Strategy to Prepare Small Water Clusters via Interacting with Functional Molecules.

Int J Mol Sci 2021 Jul 31;22(15). Epub 2021 Jul 31.

CAS Key Lab of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.

Although small water clusters (SWCs) are important in many research fields, efficient methods of preparing SWCs are still rarely reported, which is mainly due to the lack of related materials and understanding of the molecular interaction mechanisms. In this study, a series of functional molecules were added in water to obtain small water cluster systems. The decreasing rate of the half-peak width in a sodium dodecyl sulfate (SDS)-water system reaches ≈20% at 0.05 mM from O nuclear magnetic resonance (NMR) results. Based on density functional theory (DFT) and molecular dynamics (MD) simulation calculation, it can be concluded that functional molecules with stronger negative electrostatic potential (ESP) and higher hydrophilicity have a stronger ability to destroy big water clusters. Notably, the concentrations of our selected molecule systems are one to two magnitudes lower than that of previous reports. This study provides a promising way to optimize aqueous systems in various fields such as oilfield development, protein stability, and metal anti-corrosion.
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http://dx.doi.org/10.3390/ijms22158250DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8347634PMC
July 2021

Single cell imaging reveals cisplatin regulating interactions between transcription (co)factors and DNA.

Chem Sci 2021 Feb 25;12(15):5419-5429. Epub 2021 Feb 25.

Beijing National Laboratory for Molecular Sciences, CAS Research/Education Center for Excellence in Molecular Sciences, National Centre for Mass Spectrometry in Beijing, CAS Key Laboratory of Analytical Chemistry for Living Biosystems, Institute of Chemistry, Chinese Academy of Sciences Beijing 100190 People's Republic of China

Cisplatin is an extremely successful anticancer drug, and is commonly thought to target DNA. However, the way in which cisplatin-induced DNA lesions regulate interactions between transcription factors/cofactors and genomic DNA remains unclear. Herein, we developed a dual-modal microscopy imaging strategy to investigate, , the formation of ternary binding complexes of the transcription cofactor HMGB1 and transcription factor Smad3 with cisplatin crosslinked DNA in single cells. We utilized confocal microscopy imaging to map EYFP-fused HMGB1 and fluorescent dye-stained DNA in single cells, followed by the visualization of cisplatin using high spatial resolution (200-350 nm) time of flight secondary ion mass spectrometry (ToF-SIMS) imaging of the same cells. The superposition of the fluorescence and the mass spectrometry (MS) signals indicate the formation of HMGB1-Pt-DNA ternary complexes in the cells. More significantly, for the first time, similar integrated imaging revealed that the cisplatin lesions at Smad-binding elements, for example GGC(GC)/(CG) and AGAC, disrupted the interactions of Smad3 with DNA, which was evidenced by the remarkable reduction in the expression of Smad-specific luciferase reporters subjected to cisplatin treatment. This finding suggests that Smad3 and its related signalling pathway are most likely involved in the intracellular response to cisplatin induced DNA damage.
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http://dx.doi.org/10.1039/d0sc06760aDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8179581PMC
February 2021

Design of Low Bandgap CsPb Sn I Br Perovskite Solar Cells with Excellent Phase Stability.

Small 2021 Jul 23;17(30):e2101380. Epub 2021 Jun 23.

Key Laboratory of Green Printing, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences (ICCAS), Beijing Engineering Research Center of Nanomaterials for Green Printing Technology, National Laboratory for Molecular Sciences (BNLMS), Beijing, 100190, P. R. China.

Novel all-inorganic Sn-Pb alloyed perovskites are developed aiming for low toxicity, low bandgap, and long-term stability. Among them, CsPb Sn I Br is predicted as an ideal perovskite with favorable band gap, but previously is demonstrated unable to convert to perovskite phase by thermal annealing. In this report, a series of CsPb Sn I Br perovskites with tunable bandgaps from 1.92 to 1.38 eV are successfully prepared for the first time via low annealing temperature (60 °C). Compared to the pure CsPbI Br, these Sn-Pb alloyed perovskites show superior stability. Furthermore, a novel α-phase-stabilization mechanism of the inorganic Sn-Pb alloyed perovskite by reconfiguring the perovskite crystallization process with chloride doping is provided. Simultaneously, a dense protection layer is formed by the coordination reaction between the surface lead dangling bonds and sulfate ion to retard the permeation of external oxygen and moisture, leading to less oxidation of Sn in perovskite film. As a result, the fabricated all-inorganic Sn-Pb perovskite solar cells (PSCs) show a champion power conversion efficiency of 10.39% with improved phase stability and long-term ambient stability against light, heat, and humidity. This work provides a viable strategy in fabricating high-performance narrow-bandgap all-inorganic PSCs.
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http://dx.doi.org/10.1002/smll.202101380DOI Listing
July 2021

An Efficient Trap Passivator for Perovskite Solar Cells: Poly(propylene glycol) bis(2-aminopropyl ether).

Nanomicro Lett 2020 Aug 29;12(1):177. Epub 2020 Aug 29.

CAS Key Laboratory of Organic Solids, Beijing National Laboratory for Molecular Sciences, Institute of Chemistry Chinese Academy of Sciences, Beijing, 100190, People's Republic of China.

Perovskite solar cells (PSCs) are regarded as promising candidates for future renewable energy production. High-density defects in the perovskite films, however, lead to unsatisfactory device performances. Here, poly(propylene glycol) bis(2-aminopropyl ether) (PEA) additive is utilized to passivate the trap states in perovskite. The PEA molecules chemically interact with lead ions in perovskite, considerably passivate surface and bulk defects, which is in favor of charge transfer and extraction. Furthermore, the PEA additive can efficiently block moisture and oxygen to prolong the device lifetime. As a result, PEA-treated MAPbI (MA: CHNH) solar cells show increased power conversion efficiency (PCE) (from 17.18 to 18.87%) and good long-term stability. When PEA is introduced to (FAPbI)(MAPbBr) (FA: HC(NH)) solar cells, the PCE is enhanced from 19.66 to 21.60%. For both perovskites, their severe device hysteresis is efficiently relieved by PEA.
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http://dx.doi.org/10.1007/s40820-020-00517-yDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7770690PMC
August 2020

Real-Time Characterization of the Fine Structure and Dynamics of an Electrical Double Layer at Electrode-Electrolyte Interfaces.

J Phys Chem Lett 2021 Jun 1;12(22):5279-5285. Epub 2021 Jun 1.

Beijing National Laboratory for Molecular Sciences, National Centre for Mass Spectrometry in Beijing, CAS Key Laboratory of Analytical Chemistry for Living Biosystems, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.

The chemisorption of an electrolyte species on electrode surfaces is ubiquitous and affects the dynamics and mechanism of various electrochemical reactions. Understanding of the chemical structure and property of the resulting electrical double layer is vital but limited. Herein, we operando probed the electrochemical interface between a gold electrode surface and a common electrolyte, phosphate buffer, using our newly developed in situ liquid secondary ion mass spectrometry. We surprisingly found that, on the positively charged gold electrode surface, sodium cations were anchored in the Stern layer in a partially dehydrated form by a formation of compact ion pairs with the accumulated phosphate anions. The resulting strong adsorption phase was further revealed to retard the electro-oxidation reaction of ascorbate. This finding addressed one major gap in the fundamental science of electrode-electrolyte interfaces, namely, where and how cations reside in the double layer to impose effects on electrochemical reactions, providing insights into the engineering of better electrochemical systems.
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http://dx.doi.org/10.1021/acs.jpclett.1c01134DOI Listing
June 2021

Nanoparticle-mediated convection-enhanced delivery of a DNA intercalator to gliomas circumvents temozolomide resistance.

Nat Biomed Eng 2021 09 27;5(9):1048-1058. Epub 2021 May 27.

Department of Biomedical Engineering, Yale University, New Haven, CT, USA.

In patients with glioblastoma, resistance to the chemotherapeutic temozolomide (TMZ) limits any survival benefits conferred by the drug. Here we show that the convection-enhanced delivery of nanoparticles containing disulfide bonds (which are cleaved in the reductive environment of the tumour) and encapsulating an oxaliplatin prodrug and a cationic DNA intercalator inhibit the growth of TMZ-resistant cells from patient-derived xenografts, and hinder the progression of TMZ-resistant human glioblastoma tumours in mice without causing any detectable toxicity. Genome-wide RNA profiling and metabolomic analyses of a glioma cell line treated with the cationic intercalator or with TMZ showed substantial differences in the signalling and metabolic pathways altered by each drug. Our findings suggest that the combination of anticancer drugs with distinct mechanisms of action with selective drug release and convection-enhanced delivery may represent a translational strategy for the treatment of TMZ-resistant gliomas.
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http://dx.doi.org/10.1038/s41551-021-00728-7DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8497438PMC
September 2021

Electrical Loss Management by Molecularly Manipulating Dopant-free Poly(3-hexylthiophene) towards 16.93 % CsPbI Br Solar Cells.

Angew Chem Int Ed Engl 2021 Jul 21;60(30):16388-16393. Epub 2021 Jun 21.

Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.

Inorganic cesium lead halide perovskites offer a pathway towards thermally stable photovoltaics. However, moisture-induced phase degradation restricts the application of hole transport layers (HTLs) with hygroscopic dopants. Dopant-free HTLs fail to realize efficient photovoltaics due to severe electrical loss. Herein, we developed an electrical loss management strategy by manipulating poly(3-hexylthiophene) with a small molecule, i.e., SMe-TATPyr. The developed P3HT/SMe-TATPyr HTL shows a three-time increase of carrier mobility owing to breaking the long-range ordering of "edge-on" P3HT and inducing the formation of "face-on" clusters, over 50 % decrease of the perovskite surface defect density, and a reduced voltage loss at the perovskite/HTL interface because of favorable energy level alignment. The CsPbI Br perovskite solar cell demonstrates a record-high efficiency of 16.93 % for dopant-free HTL, and superior moisture and thermal stability by maintaining 96 % efficiency at low-humidity condition (10-25 % R. H.) for 1500 hours and over 95 % efficiency after annealing at 85 °C for 1000 hours.
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http://dx.doi.org/10.1002/anie.202105176DOI Listing
July 2021

Fluorescence live cell imaging revealed wogonin targets mitochondria.

Talanta 2021 Aug 23;230:122328. Epub 2021 Mar 23.

Beijing National Laboratory for Molecular Sciences, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, People's Republic of China; University of Chinese Academy of Sciences, Beijing, 100049, People's Republic of China; Basic Medical College, Shandong University of Traditional Chinese Medicine, Jinan, 250355, PR China; National Centre for Mass Spectrometry in Beijing, China. Electronic address:

Scutellaria baicalensis is one of the widely used Chinese traditional medicines, and wogonin is one of major active components in it. However, the mechanism of action of wogonin has largely remained unclear. In this work, we designed a fluorescent probe, namely ATTO565-WGN, by conjugating wogonin with the fluorophore ATTO565 based on Mannich reaction via a flexible chain linker. In vitro assays verified that the ATTO565-WGN conjugate has a similar anti-proliferative activity to wogonin against human A549 and HeLa cancer cell lines. Combining co-localization and competition studies, confocal fluorescence imaging clearly demonstrated that the fluorescent wogonin probe predominantly located in mitochondrial area of living cells, indicating that wogonin acts at mitochondrion to exert its pharmacological functions. Significantly, the conjugated ATTO565 fluorophore conferred the wogonin probe STED (Stimulated Emission Depletion) feature, enabling STED fluorescence living cell imaging with a 55 nm of ultrahigh spatial resolution. This will greatly beneficial for the in situ investigation of interactions between wogonin and biological targets at the finely organized and dynamic mitochondria of living cells. Moreover, this work also provides novel insights into rational design of mitochondrion targeting fluorescence probes for ultrahigh resolution living cell imaging.
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http://dx.doi.org/10.1016/j.talanta.2021.122328DOI Listing
August 2021

A Near-Infrared-II Polymer with Tandem Fluorophores Demonstrates Superior Biodegradability for Simultaneous Drug Tracking and Treatment Efficacy Feedback.

ACS Nano 2021 03 9;15(3):5428-5438. Epub 2021 Mar 9.

Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Polymer Physics and Chemistry, Institute of Chemistry Chinese Academy of Sciences, Beijing 100190, China.

NIR-II (1000-1700 nm) fluorescence imaging is continually attracting strong research interest. However, current NIR-II imaging materials are limited to small molecules with fast blood clearance and inorganic nanomaterials and organic conjugated polymers of poor biodegradability and low biocompatibility. Here, we report a highly biodegradable polyester carrying tandem NIR-II fluorophores as a promising alternative. The polymer encapsulated a platinum intercalator (56MESS, (5,6-dimethyl-1,10-phenanthroline) (1,2-diaminocyclohexane) platinum(II)) and was conjugated with both a cell-targeting RGD peptide and a caspase-3 cleavable peptide probe to form nanoparticles for simultaneous NIR-II and apoptosis imaging. , the nanoparticles were approximately 4-1000- and 1.5-10-fold more potent than cisplatin and 56MESS, respectively. Moreover, , they significantly inhibited tumor growth on a multidrug-resistant patient-derived mouse model (PDX). Finally, through label-free laser desorption-ionization mass spectrometry imaging (MALDI-MSI), 56MESS release in the deeper tumors was observed. This work highlighted the use of biodegradable NIR-II polymers for monitoring drugs and therapeutic effect feedback in real-time.
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http://dx.doi.org/10.1021/acsnano.1c00076DOI Listing
March 2021

Open-flow microperfusion combined with mass spectrometry for in vivo liver lipidomic analysis.

Analyst 2021 Mar 22;146(6):1915-1923. Epub 2021 Jan 22.

Beijing National Laboratory for Molecular Sciences, CAS Research/Education Center for Excellence in Molecular Sciences, Key Laboratory of Analytical Chemistry for Living Biosystems, Institute of Chemistry Chinese Academy of Sciences, Beijing Mass Spectrum Center, Beijing 100190, China.

At present, conventional microdialysis (MD) techniques cannot efficiently sample lipids in vivo, possibly due to the high mass transfer resistance and/or the serious adsorption of lipids onto the semi-permeable membrane of a MD probe. The in vivo monitoring of lipids could be of great significance for the study of disease development and mechanisms. In this work, an open-flow microperfusion (OFM) probe was fabricated, and the conditions for sampling lipids via OFM were optimized. Using OFM, the recovery of lipid standards was improved to more than 34.7%. OFM is used for the in vivo sampling of lipids in mouse liver tissue with fibrosis, and it is then combined with mass spectrometry (MS) to perform lipidomic analysis. 156 kinds of lipids were identified in the dialysate collected via OFM, and it was found that the phospholipid levels, including PC, PE, and SM, were significantly higher in a liver suffering from fibrosis. For the first time, OFM combined with MS to sample and analyze lipids has provided a promising platform for in vivo lipidomic studies.
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http://dx.doi.org/10.1039/d0an02189jDOI Listing
March 2021

Mechanistic Insight into Royal Protein Inhibiting the Gram-Positive Bacteria.

Biomolecules 2021 01 6;11(1). Epub 2021 Jan 6.

Institute of Apicultural Research/Key Laboratory of Pollinating Insect Biology, Ministry of Agriculture and Rural Affairs, Chinese Academy of Agricultural Sciences, Beijing 100093, China.

Royal jelly (RJ), a natural honeybee product, has a wide range of antibacterial activities. N-glycosylated major royal jelly protein 2 (N-MRJP2), purified from RJ, can inhibit the growth of (, Gram-positive), a contagious etiological agent of the American foulbrood disease of honeybees. However, the inhibitory mechanism is largely unknown. Antibacterial assay and membrane proteome were conducted to investigate the inhibition capacity of RJ from different instar larvae and treated by N-MRJP2, respectively. The similar antibacterial efficiency of RJ from different larval instar indicates that RJ is vital for the adaptive immune defense of small larvae. The killing of by N-MRJP2 is achieved by disturbing the cell wall biosynthesis, increasing the permeability of cell membrane, hindering aerobic respiration, restraining cell division and inducing cell death. This demonstrates that RJ is critical for the passive immunity of immature larvae and N-MRJP2 can be used as natural antibiotic substance to resist , even for other gram-positive bacteria. This constitutes solid evidence that RJ and N-MRJP2 have potentials as novel antibacterial agents.
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http://dx.doi.org/10.3390/biom11010064DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7825125PMC
January 2021

Breaking the Intracellular Redox Balance with Diselenium Nanoparticles for Maximizing Chemotherapy Efficacy on Patient-Derived Xenograft Models.

ACS Nano 2020 Dec 7. Epub 2020 Dec 7.

Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Polymer Physics and Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.

Excessive oxidative stress in cancer cells can induce cancer cell death. Anticancer activity and drug resistance of chemotherapy are closely related to the redox state of tumor cells. Herein, five lipophilic Pt(IV) prodrugs were synthesized on the basis of the most widely used anticancer drug cisplatin, whose anticancer efficacy and drug resistance are closely related to the intracellular redox state. Subsequently, a series of cisplatin-sensitive and drug-resistant cell lines as well as three patient-derived primary ovarian cancer cells have been selected to screen those prodrugs. To verify if the disruption of redox balance can be combined with these Pt(IV) prodrugs, we then synthesized a polymer with a diselenium bond in the main chain for encapsulating the most effective prodrug to form nanoparticles (NP(Se)s). NP(Se)s can efficiently break the redox balance simultaneously depleting GSH and augmenting ROS, thereby achieving a synergistic effect with cisplatin. In addition, genome-wide analysis RNA-seq was employed to provide a comprehensive understanding of the changes in transcriptome and the alterations in redox-related pathways in cells treated with NP(Se)s and cisplatin. Thereafter, patient-derived xenograft models of hepatic carcinoma (PDX) and multidrug-resistant lung cancer (PDX) were established to evaluate the therapeutic effect of NP(Se)s, and a significant antitumor effect was achieved on both models with NP(Se)s. Overall, this study provides a promising strategy to break the redox balance for maximizing the efficacy of platinum-based cancer therapy.
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http://dx.doi.org/10.1021/acsnano.0c06190DOI Listing
December 2020

Photoactivatable diazido Pt(IV) anticancer complex can bind to and oxidize all four nucleosides.

Dalton Trans 2020 Dec;49(47):17157-17163

Key Laboratory of Hubei Province for Coal Conversion and New Carbon Materials; School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan 430081, P. R. China.

Photoactivatable diazidodihydroxido Pt(iv) complex trans,trans,trans-[Pt(N3)2(OH)2(py)2] (1; py = pyridine) is a promising anticancer agent which can be activated by visible light to induce cancer cell death. DNA has been thought to be involved in the mechanism of action of this kind of Pt(iv) prodrug. However, the detailed photodecomposition pathways of complex 1 and its interaction modes with DNA are complex. Herein we report that upon light irradiation complex 1 can bind to all four nucleosides covalently with the reduced Pt(ii) species. Moreover, apart from the covalent coordination, various oxidation adducts of these four nucleosides induced by the reactive oxidative species (ROS) generated during the photoactivation of the complex 1 have also been identified, especially the induced oxidation of adenosine and cytidine which was firstly reported for this kind of photoactivatable Pt(iv) prodrug. Such dual-action may contribute to the highly potent photo-antiproliferativity of complex 1 towards cancer cells, which may account for the unique mechanism of action of the photoactivatable diazido Pt(iv) anticancer complexes.
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http://dx.doi.org/10.1039/d0dt03090bDOI Listing
December 2020

Visualization of Proteins in Single Cells by Time-of-Flight-Secondary Ion Mass Spectrometry Coupled with Genetically Encoded Chemical Tags.

Anal Chem 2020 12 17;92(23):15517-15525. Epub 2020 Nov 17.

Beijing National Laboratory for Molecular Sciences, National Centre for Mass Spectrometry in Beijing, CAS Key Laboratory of Analytical Chemistry for Living Biosystems, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, People's Republic of China.

visualization of proteins of interest in single cells is attractive in cell biology, molecular biology, and biomedicine fields. Time-of-flight-secondary ion mass spectrometry (ToF-SIMS) is a powerful tool for imaging small organic molecules in single cells, yet difficult to image biomacromolecules such as proteins and DNA. Herein, a universal strategy is reported to image specific proteins in single cells by ToF-SIMS following genetic incorporation of fluorine-containing unnatural amino acids as a chemical tag into the proteins a genetic code expansion technique. The method was developed and validated by imaging a green fluorescence protein (GFP) in and human HeLa cancer cells and then utilized to visualize the characteristic polar distribution of chemotaxis protein CheA in cells and the interaction between high-mobility group box 1 protein and cisplatin-damaged DNA in HeLa cells. The present work highlights the power of ToF-SIMS imaging combined with genetically encoded chemical tags for visualization of specific proteins as well as the interactions between proteins and drugs or drug-damaged DNA in single cells.
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http://dx.doi.org/10.1021/acs.analchem.0c03448DOI Listing
December 2020

Near-Infrared Light Irradiation Induced Mild Hyperthermia Enhances Glutathione Depletion and DNA Interstrand Cross-Link Formation for Efficient Chemotherapy.

ACS Nano 2020 11 21;14(11):14831-14845. Epub 2020 Oct 21.

Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Polymer Physics and Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.

DNA alkylating agents generally kill tumor cells by covalently binding with DNA to form interstrand or intrastrand cross-links. However, in the case of cisplatin, only a few DNA adducts (<1%) are highly toxic irreparable interstrand cross-links. Furthermore, cisplatin is rapidly detoxified by high levels of intracellular thiols such as glutathione (GSH). Since the discovery of its mechanism of action, people have been looking for ways to directly and efficiently remove intracellular GSH and increase interstrand cross-links to improve drug efficacy and overcome resistance, but there has been little breakthrough. Herein, we hypothesized that the anticancer efficiency of cisplatin can be enhanced through iodo-thiol click chemistry mediated GSH depletion and increased formation of DNA interstrand cross-links mild hyperthermia triggered by near-infrared (NIR) light. This was achieved by preparing an amphiphilic polymer with platinum(IV) (Pt(IV)) prodrugs and pendant iodine atoms (iodides). The polymer was further used to encapsulate IR780 and assembled into Pt-I-IR780 nanoparticles. Induction of mild hyperthermia (43 °C) at the tumor site by NIR light irradiation had three effects: (1) it accelerated the GSH-mediated reduction of Pt(IV) in the polymer main chain to platinum(II) (Pt(II)); (2) it boosted the iodo-thiol substitution click reaction between GSH and iodide, thereby attenuating the GSH-mediated detoxification of cisplatin; (3) it increased the proportion of highly toxic and irreparable Pt-DNA interstrand cross-links. Therefore, we find that mild hyperthermia induced NIR irradiation can enhance the killing of cancer cells and reduce the tumor burden, thus delivering efficient chemotherapy.
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http://dx.doi.org/10.1021/acsnano.0c03781DOI Listing
November 2020

Reactions of a photoactivatable diazido Pt(iv) anticancer complex with a single-stranded oligodeoxynucleotide.

Dalton Trans 2020 Aug;49(32):11249-11259

Key Laboratory of Hubei Province for Coal Conversion and New Carbon Materials; School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan 430081, P. R. China.

Platinum based anticancer agents are widely applied in clinic and their major target is believed to be DNA. Herein, the interaction of a photoactivatable diazido Pt(iv) anticancer prodrug trans,trans,trans-[Pt(N3)2(OH)2(py)2] (py = pyridine; 1) with a 15-mer single-G-containing oligodeoxynucleotide (ODN I: 5'-CT2CTCTTG8T9CT11TCTC-3') was investigated by mass spectrometric methods. Up to penta-platinated ODN I adducts were identified from primary mass spectra while the mono- and di-platinated adducts had the highest intensity. Fragmentation of mono-, di- and tri-platinated I adducts in tandem MS revealed that T2, G8, T11 and T9 are binding sites. No cytosine sites were identified which may be due to the facile loss of Pt adducts from cytosine during CID. The intensity of {Pt(py)2}-bound adducts was comparable to that of {Pt(N3)(py)2}-bound adducts, indicating that the photo-reduction pathway of complex 1 from Pt(iv) to Pt(ii) through two one-electron donations from two azides was substantial. Moreover, no transformation of N3 to NH3 on the {Pt(N3)(py)2}-bound adducts was observed, whereas it is very popular during the reactions of complexes with short ODNs or mono-nucleotides. The oxidation on I induced by the reactive oxygen species (ROS) formed by the photodecomposition of complex 1 was significant, and the oxidation of G8 to 8-hydroxyguanine (8-OH-G), spiroiminodihydantoin (Sp) and 2,6-diamino-4-hydroxy-5-formamidopyrimidine (FapyG) was discovered. These results unambiguously revealed a sequence-length-dependent photochemical reactivity of complex 1 when it interacted with different ODNs, providing deeper understanding in the reactivity of photoactivatable diazido anticancer Pt(iv) prodrugs to DNA.
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http://dx.doi.org/10.1039/d0dt02208jDOI Listing
August 2020

Bio-inspired vertebral design for scalable and flexible perovskite solar cells.

Nat Commun 2020 06 15;11(1):3016. Epub 2020 Jun 15.

College of Chemistry, Nanchang University, 999 Xuefu Avenue, Nanchang, 330031, China.

The translation of unparalleled efficiency from the lab-scale devices to practical-scale flexible modules affords a huge performance loss for flexible perovskite solar cells (PSCs). The degradation is attributed to the brittleness and discrepancy of perovskite crystal growth upon different substrates. Inspired by robust crystallization and flexible structure of vertebrae, herein, we employ a conductive and glued polymer between indium tin oxide and perovskite layers, which simultaneously facilitates oriented crystallization of perovskite and sticks the devices. With the results of experimental characterizations and theoretical simulations, this bionic interface layer accurately controls the crystallization and acts as an adhesive. The flexible PSCs achieve the power conversion efficiencies of 19.87% and 17.55% at effective areas of 1.01 cm and 31.20 cm respectively, retaining over 85% of original efficiency after 7000 narrow bending cycles with negligible angular dependence. Finally, the modules are assembled into a wearable solar-power source, enabling the upscaling of flexible electronics.
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http://dx.doi.org/10.1038/s41467-020-16831-3DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7295992PMC
June 2020

Unexpected Thymine Oxidation and Collision-Induced Thymine-Pt-guanine Cross-Linking on 5'-TpG and 5'-GpT by a Photoactivatable Diazido Pt(IV) Anticancer Complex.

Inorg Chem 2020 Jun 25;59(12):8468-8480. Epub 2020 May 25.

Beijing National Laboratory for Molecular Sciences; National Centre for Mass Spectrometry in Beijing; CAS Key Laboratory of Analytical Chemistry for Living Biosystems, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China.

The photochemical products of dinucleotides 5'-TpG/5'-GpT with a photoactivatable anticancer Pt(IV) complex (,,-[Pt(N)(OH)(py)], py = pyridine; ) were characterized by electrospray ionization mass spectrometry. The primary MS showed the main products were monoplatinated and diplatinated adducts for both the dinucleotides accompanied by the formation of minor triplatinated dinucleotides, indicating that T-N3 and G-N1 may be platination sites additional to the well-known G-N7 site. Surprisingly, a series of minor platinated adducts with oxidation of guanine and/or thymine were observed. Although guanine is more sensitive to oxidation than thymine, thymine can compete with guanine for complex -induced oxidation, of which the oxidation adducts were identified as - and -diastereomers of 5,6-dihydroxy-5,6-dihydrothymidine (,-ThdGly), 5-formyl-2'-deoxyuridine (5-FormdUrd), and 5-(hydroxymethyl)-2'-deoxyuridine (5-HMdUrd), respectively. While for guanine, apart from 8-hydroxyguanine (8-OH-G) and -formylamidoiminohydantoin (RedSp), other guanine oxidized adducts such as spiroiminodihydantoin (Sp), dehydroguanidinohydantoin (DGh), and 2,6-diamino-4-hydroxy-5-formamidopyrimidine (FapyG) were also identified. MS/MS analysis showed that unique fragments with a Pt moiety [Pt(N)(py)] cross-linking the G and T bases were formed during the fragmentation of monoplatinated dinucleotides. Such binding mode to and oxidative damages on DNA bases imposed by the diazido Pt(IV) complex are apparently distinct from those of cisplatin, perhaps accounting for its unique mechanism of action.
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http://dx.doi.org/10.1021/acs.inorgchem.0c00894DOI Listing
June 2020

Platinum(II) Terpyridine Anticancer Complexes Possessing Multiple Mode of DNA Interaction and EGFR Inhibiting Activity.

Front Chem 2020 28;8:210. Epub 2020 Apr 28.

Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Analytical Chemistry for Living Biosystems, Beijing Centre for Mass Spectrometry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, China.

Platinum(II) terpyridine complexes has attracted increasing attention as they have displayed great potential as antitumor agents due to their high intercalation affinity with nucleic acids. Epidermal growth factor receptor (EGFR) is often overexpressed in various tumor cells, leading to uncontrolled growth of tumor, and is regarded as an important target for developing novel antitumor drugs. Herein, we report four platinum(II) terpyridine complexes bearing EGFR inhibiting 4-anilinoquinazoline derivatives as potent multi-targeting antiproliferation agents against a series of cancer cells. EGFR inhibition assay revealed that these complexes are highly potent EGFR inhibitors. But competitive DNA binding assay and docking simulations also suggested that these complexes exhibited multiple modes of DNA interaction, especially great affinity toward DNA minor groove. Finally, cellular uptake and distribution measurements by inductively coupled plasma mass spectrometry (ICP-MS) and time-of-flight secondary ion mass spectrometry (ToF-SIMS) demonstrated that both nucleus DNA and membrane proteins are important targets for their anticancer mechanisms. The complexes herein can therefore be regarded as promising multi-targeting anticancer agents.
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http://dx.doi.org/10.3389/fchem.2020.00210DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7199514PMC
April 2020

Ion Exchange/Insertion Reactions for Fabrication of Efficient Methylammonium Tin Iodide Perovskite Solar Cells.

Adv Sci (Weinh) 2020 May 14;7(9):1903047. Epub 2020 Mar 14.

Key Laboratory of Green Printing Institute of Chemistry Chinese Academy of Sciences Beijing 100190 P. R. China.

The low toxicity, narrow bandgaps, and high charge-carrier mobilities make tin perovskites the most promising light absorbers for low-cost perovskite solar cells (PSCs). However, the development of the Sn-based PSCs is seriously hampered by the critical issues of poor stability and low power conversion efficiency (PCE) due to the facile oxidation of Sn to Sn and poor film formability of the perovskite films. Herein, a synthetic strategy is developed for the fabrication of methylammonium tin iodide (MASnI) film via ion exchange/insertion reactions between solid-state SnF and gaseous methylammonium iodide. In this way, the nucleation and crystallization of MASnI can be well controlled, and a highly uniform pinhole-free MASnI perovskite film is obtained. More importantly, the detrimental oxidation can be effectively suppressed in the resulting MASnI film due to the presence of a large amount of remaining SnF. This high-quality perovskite film enables the realization of a PCE of 7.78%, which is among the highest values reported for the MASnI-based solar cells. Moreover, the MASnI solar cells exhibit high reproducibility and good stability. This method provides new opportunities for the fabrication of low-cost and lead-free tin-based halide perovskite solar cells.
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http://dx.doi.org/10.1002/advs.201903047DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7201265PMC
May 2020

Advances in Toxicological Research of the Anticancer Drug Cisplatin.

Chem Res Toxicol 2019 08 5;32(8):1469-1486. Epub 2019 Aug 5.

Beijing National Laboratory for Molecular Sciences; National Centre for Mass Spectrometry in Beijing; CAS Key Laboratory of Analytical Chemistry for Living Biosystems , Institute of Chemistry, Chinese Academy of Sciences , Beijing 100190 , P.R. China.

Cisplatin is one of the most widely used chemotherapeutic agents for various solid tumors in the clinic due to its high efficacy and broad spectrum. The antineoplastic activity of cisplatin is mainly due to its ability to cross-link with DNA, thus blocking transcription and replication. Unfortunately, the clinical use of cisplatin is limited by its severe, dose-dependent toxic side effects. There are approximately 40 specific toxicities of cisplatin, among which nephrotoxicity is the most common one. Other common side effects include ototoxicity, neurotoxicity, gastrointestinal toxicity, hematological toxicity, cardiotoxicity, and hepatotoxicity. These side effects together reduce the life quality of patients and require lowering the dosage of the drug, even stopping administration, thus weakening the treatment effect. Few effective measures exist clinically against these side effects because the exact mechanisms of various side effects from cisplatin remain still unclear. Therefore, substantial effort has been made to explore the complicated biochemical processes involved in the toxicology of cisplatin, aiming to identify effective ways to reduce or eradicate its toxicity. This review summarizes and reviews the updated advances in the toxicological research of cisplatin. We anticipate to provide insights into the understanding of the mechanisms underlying the side effects of cisplatin and designing comprehensive therapeutic strategies involving cisplatin.
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http://dx.doi.org/10.1021/acs.chemrestox.9b00204DOI Listing
August 2019

Discovery of Cisplatin Binding to Thymine and Cytosine on a Single-Stranded Oligodeoxynucleotide by High Resolution FT-ICR Mass Spectrometry.

Molecules 2019 May 14;24(10). Epub 2019 May 14.

Beijing National Laboratory for Molecular Sciences, National Centre for Mass Spectrometry in Beijing, CAS Key Laboratory of Analytical Chemistry for Living Biosystems, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.

The clinically widely-used anticancer drug, cisplatin, binds strongly to DNA as a DNA-damaging agent. Herein, we investigated the interaction of cisplatin with a 15-mer single-stranded C,T-rich oligodeoxynucleotide, 5'-CCTTCTTGCTTCTCC-3' (ODN15), using ultra-high resolution Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) in conjunction with tandem mass spectrometry (top-down MS). Top-down MS analysis with collision-induced dissociation (CID) fragmentation of the mono-platinated and di-platinated ODN15 provided abundant and informative Pt-containing or Pt-free a/[a - B], w and internal fragments, allowing the unambiguous identification of T, T, C, and T as the platination sites on the cisplatin-ODN15 adducts. These results revealed that, in addition to the well-established guanine site, the unexpected thermodynamic binding of cisplatin to cytosine and thymine bases was also evident at the oligonucleotide level. Furthermore, the binding models of cisplatin with cytosine and thymine bases were built as the Pt coordinated to cytosine-N(3) and thymine-N(3) with displacement of the proton or tautomerization of thymine. These findings contribute to a better understanding of the mechanism of action of cisplatin and its preference for gene loci when the drug binds to cellular DNA, and also demonstrate the great potential and superiority of FT-ICR MS in studying the interactions of metallodrugs with large biomolecules.
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http://dx.doi.org/10.3390/molecules24101852DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6571787PMC
May 2019

Sub-10 nm Ag Nanoparticles/Graphene Oxide: Controllable Synthesis, Size-Dependent and Extremely Ultrahigh Catalytic Activity.

Small 2019 06 26;15(23):e1901701. Epub 2019 Apr 26.

Beijing National Laboratory for Molecular Science, CAS Research/Education Center for Excellence in Molecular Sciences, CAS Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.

While tremendous advancements in Ag nanoparticle (AgNP)-based materials have been made, the development of a facile protocol for preparing sub-10 nm AgNPs with controllable size and ultrahigh performance remains a formidable challenge. It is shown that AgNPs/graphene oxide (AgNPs/GO) bearing 2.5, 4.3, and 6.2 nm AgNPs (2.5-AgNPs/GO, 4.3-AgNPs/GO, and 6.2-AgNPs/GO, respectively) could be fabricated via light-induced synthesis. Their catalytic activity toward 4-nitrophenol (4-NP) reduction, which is a "gold standard" for evaluating the performance of noble metal-based catalysts, is studied. When normalized by mole and area, the activity exhibits an order of 4.3-AgNPs/GO > 6.2-AgNPs/GO > 2.5-AgNPs/GO and 6.2-AgNPs/GO > 4.3-AgNPs/GO > 2.5-AgNPs/GO, respectively. This trend is a result of GO-induced electron concentration reduction with decreasing AgNP size. Significantly, under similar conditions, the activity of 4.3-AgNPs/GO is substantially superior to that of numerous state-of-the-art noble metal-based catalysts. The ultrafine size of the AgNPs and their surface accommodation on the unobstructed 2D GO scaffolds without capping reagents/covers, which make the abundantly exposed catalytically active sites highly accessible to substrate molecules, play an important role in their extremely ultrahigh performance. This work paves a new avenue for high-performance AgNP-based materials, and by taking 4-NP reduction as a proof-of-concept, provides new scientific insights into the rational design of surface-based advanced materials.
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http://dx.doi.org/10.1002/smll.201901701DOI Listing
June 2019

Proteomic Strategy for Identification of Proteins Responding to Cisplatin-Damaged DNA.

Anal Chem 2019 05 24;91(9):6035-6042. Epub 2019 Apr 24.

Beijing National Laboratory for Molecular Sciences; National Centre for Mass Spectrometry in Beijing; CAS Key Laboratory of Analytical Chemistry for Living Biosystems , Institute of Chemistry, Chinese Academy of Sciences , Beijing 100190 , P. R. China.

A new proteomic strategy combining functionalized magnetic nanoparticle affinity probes with mass spectrometry was developed to capture and identify proteins specifically responding to 1,2-d(GpG) intrastrand cisplatin-cross-linked DNA, the major DNA lesion caused by cisplatin and thought to induce apoptosis. A 16-mer oligodeoxynucleotide (ODN) duplex and its cisplatin-cross-linked adduct were immobilized on magnetic nanoparticles via click reaction, respectively, to fabricate negative and positive affinity probes which were very stable in cellular protein extracts due to the excellent bio-orthogonality of click chemistry and the inertness of covalent triazole linker. Quantitative mass spectrometry results unambiguously revealed the predominant binding of HMGB1 and HMGB2, the well-established specific binders of 1,2-cisplatin-cross-linked DNA, to the cisplatin-cross-linked ODN, thus validating the accuracy and reliability of our strategy. Furthermore, 5 RNA or single-stranded DNA binding proteins, namely, hnRNP A/B, RRP44, RL30, RL13, and NCL, were demonstrated to recognize specifically the cisplatinated ODN, indicating the significantly unwound ODN duplex by cisplatin cross-linking. In contrast, the binding of a transcription factor TFIIFa to DNA was retarded due to cisplatin damage, implying that the cisplatin lesion stalls DNA transcription. These findings promote understanding in the cellular responses to cisplatin-damaged DNA and inspire further precise elucidation of the action mechanism of cisplatin.
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http://dx.doi.org/10.1021/acs.analchem.9b00554DOI Listing
May 2019

In Situ Liquid Secondary Ion Mass Spectrometry: A Surprisingly Soft Ionization Process for Investigation of Halide Ion Hydration.

Anal Chem 2019 06 17;91(11):7039-7046. Epub 2019 Apr 17.

Environmental Molecular Sciences Laboratory , Pacific Northwest National Laboratory , Richland , Washington 99354 , United States.

The understanding of ion solvation phenomena is of significance due to their influences on many important chemical, biological, and environmental processes. Mass spectrometry (MS)-based methods have been used to investigate this topic with molecular insights. As ion-solvent interactions are weak, ionization processes should be as soft as possible in order to retain solvation structures. An in situ liquid secondary ion MS (SIMS) approach developed in our group has been recently utilized in investigations of Li ion solvation in nonaqueous solution, and it detected a series of solvated Li ions. As traditionally SIMS has long been recognized as a hard ionization process with strong damage occurring at the sputtering interface, it is very interesting to study further how soft in situ liquid SIMS can be. In this work, we used halide ion hydration as an example to compare the ionization performance of the in situ liquid SIMS approach with regular electrospray ionization MS (ESI-MS). Results show that, although ESI has been recognized as a soft ionization method, nearly no solvated halide ions were detected by ESI-MS analysis, which acquired only strong signals of salt ion clusters. In contrast, in liquid SIMS spectra, a series of obvious hydrated halide ion compositions could be observed. We further evaluated the hydration numbers of halide ions and revealed the effects of the ion size, charge density, and polarizability on the hydration phenomenon. Our findings demonstrated that the in situ liquid SIMS approach is surprisingly soft, and it is expected to have very broad applications on investigation of various ion-solvent interactions and many other interesting chemical processes (e.g., the initial nucleation of nanoparticle formation) in liquid environment.
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http://dx.doi.org/10.1021/acs.analchem.8b05804DOI Listing
June 2019

Mass spectrometric quantification of the binding ratio of metal-based anticancer complexes with protein thiols.

Rapid Commun Mass Spectrom 2019 May;33(10):951-958

Beijing National Laboratory for Molecular Sciences; National Centre for Mass Spectrometry in Beijing; CAS Research/Education Centre for Excellence in Molecular Sciences; CAS Key Laboratory of Analytical Chemistry for Living Biosystems, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.

Rationale: The binding ratio of metal complexes with cysteinyl thiols in proteins plays an important role in deciphering the mechanisms of action of therapeutic metal complexes, but its analysis is still a significant challenge. In this work, a quantitative mass spectrometry method is developed to determine the binding ratio of metal-based anticancer complexes with cysteines in human copper chaperone protein Atox1.

Methods: A novel strategy based on a thiol-specific stable isotopic labelling reagent was developed to determine the binding ratio of metal-based anticancer complexes, namely cisplatin and organometallic ruthenium complex [(η -biphenyl)RuCl(en)]PF (en = ethylenediamine), with the cysteinyl residues of Atox1.

Results: Both cisplatin and the ruthenium complex were reactive not only to Cys15 and/or Cys18, the copper(I) binding site of Atox1, but also to Cys44. The binding ratios of the ruthenium complex with the cysteinyl residues were much higher than those of cisplatin. However, the addition of copper(I) could markedly increase the binding ratios of cysteinyl residues of Atox1 with cisplatin, but not with the ruthenium complex.

Conclusions: This strategy can not only precisely determine the binding ratios of metal complexes to protein thiols, but also be helpful in distinguishing thiol-binding sites from other binding sites of metal complexes in proteins. We expect wide application of this method to the research of covalent/coordinative interactions between metal complexes and protein thiols.
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http://dx.doi.org/10.1002/rcm.8423DOI Listing
May 2019
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