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platinum on nitrogen doped graphene and tungsten carbide supports for ammonia electro-oxidation reaction

Frontiers of Chemical Science and Engineering 2022年第6期16卷 930-938页

作者： Kumar Siddharth Yian Wang Jing Wang Fei Xiao Gabriel Sikukuu Nambafu Usman Bin Shahid Fei Yang Ernest Pahuyo Delmo Minhua Shao Department of Chemical and Biological Engineering The Hong Kong University of Science and TechnologyHong KongChina Department of Materials Science and Engineering South University of Science and Technology of ChinaShenzhen 518055China Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou) The Hong Kong University of Science and TechnologyHong KongChina Chinese National Engineering Research Center for Control&Treatment of Heavy Metal Pollution The Hong Kong University of Science and TechnologyHong KongChina

Ammonia electrooxidation reaction involving multistep electron-proton transfer is a significant reaction for fuel cells,hydrogen production and understanding nitrogen cycle.platinum has been established as the best electrocatalyst for ammonia oxidation in aqueous alkaline media.In this study,Pt/nitrogen-doped graphene(NDG)and Pt/tungsten monocarbide(WC)/NDG are synthesized by a wet chemistry method and their ammonia oxidation activities are compared to commercial Pt/C.Pt/NDG exhibits a specific activity of 0.472 mA·cm^(-2),which is 44%higher than commercial Pt/C,thus establishing NDG as a more effective support than carbon black.Moreover,it is demonstrated that WC as a support also impacts the activity with further 30%increase in comparison to NDG.Surface modification with Ir resulted in the best electro-catalytic activity with Pt-IrAVC/NDG having almost thrice the current density of commercial Pt/C.This work adds insights regarding the role of NDG and WC as efficient supports along with significant impact of Ir surface modification.

关键词： Ammonia electro-oxidation reaction electrocatalyst supports platinum nitrogen doped graphene tungsten carbide

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platinum complexes of curcumin delivered by dual-responsive polymeric nanoparticles improve chemotherapeutic efficacy based on the enhanced anti-metastasis activity and reduce side effects

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Acta Pharmaceutica Sinica B 2020年第6期10卷 1106-1121页

作者： Yan Chen Chen Chen Xiaojuan Zhang Chuanchuan He Pengxuan Zhao Minsi Li Ting Fan Ruicong Yan Yao Lu Robert J.Lee Muhammad Waseem Khan Muhammad Sarfraz Xiang Ma Tan Yang Guangya Xiang School of Pharmacy Tongji Medical CollegeHuazhong University of Science and TechnologyWuhan 430030China College of Pharmacy the Ohio State UniversityColumbusOH 43210USA

platinum-based chemotherapy is used for non-small cell lung cancer(NSCLC).However,it has side effects and minimum efficacy against lung cancer metastasis.In this study,platinum-curcumin complexes were loaded into pH and redox dual-responsive nanoparticles(denoted as Pt-CUR@PSPPN)to facilitate intracellular release and synergistic anti-cancer effects.Pt-CUR@PSPPN was prepared by a nano-precipitation method and had a diameter of^100 nm.The nanoparticles showed increased anticancer effects both in vivo and in vitro.In addition,Pt-CUR@PSPPN blocked PI3K/AKT signal transduction pathway and inhibited MMP2 and VEGFR2,resulting in enhanced anti-metastatic activity.Furthermore,reduced side effects were also observed.In conclusion,Pt-CUR@PSPPN provided a novel and attractive therapeutic strategy for NSCLC.

关键词： platinum Curcumin Complex Nanoparticles Non-small cell lung cancer Anti-metastasis Drug delivery

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Association between homologous recombination deficiency and outcomes with platinum and platinum-free chemotherapy in patients with triple-negative breast cancer

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Cancer Biology & Medicine 2023年第2期20卷 155-168页

作者： Yimeng Chen Xue Wang Feng Du Jian Yue Yiran Si Xiaochen Zhao Lina Cui Bei Zhang Ting Bei Binghe Xu Peng Yuan Department of Medical Oncology and Clinical Trial Center National Cancer Center/National Clinical Research Center for Cancer/Cancer HospitalChinese Academy of Medical Sciences and Peking Union Medical CollegeBeijing 100021China Department of VIP Medical Services National Cancer Center/National Clinical Research Center for Cancer/Cancer HospitalChinese Academy of Medical Sciences and Peking Union Medical CollegeBeijing 100021China The Medical Department 3D Medicines Inc.Shanghai 201114China

Objective:The choice of chemotherapeutic regimen for triple-negative breast cancer(TNBC)remains controversial.Homologous recombination deficiency(HRD)has attracted increasing attention in informing chemotherapy treatment.This study was aimed at investigating the feasibility of HRD as a clinically actionable biomarker for platinum-containing and platinum-free therapy.Methods:Chinese patients with TNBC who received chemotherapy between May 1,2008 and March 31,2020 were retrospectively analyzed with a customized 3D-HRD panel.HRD positivity was defined by an HRD score≥30 or deleterious BRCA1/2 mutation.A total of 386 chemotherapy-treated patients with TNBC were screened from a surgical cohort(NCT01150513)and a metastatic cohort,and 189 patients with available clinical and tumor sequencing data were included.Results:In the entire cohort,49.2%(93/189)of patients were identified as HRD positive(40 with deleterious BRCA1/2 mutations and 53 with BRCA1/2 intact with an HRD score of≥30).In the first-line metastatic setting,platinum therapy was associated with longer median progression-free survival(mPFS)than platinum-free therapy[9.1 vs.3.0 months;hazard ratio(HR),0.43;95%confidence interval 0.22–0.84;P=0.01].Among HRD-positive patients,the mPFS was significantly longer in those treated with platinum rather than platinum-free therapy(13.6 vs.2.0 months;HR,0.11;P=0.001).Among patients administered a platinum-free regimen,HRD-negative patients showed a PFS significantly superior to that of HRD-positive patients(P=0.02;treatment-biomarker P-interaction=0.001).Similar results were observed in the BRCA1/2-intact subset.In the adjuvant setting,HRD-positive patients tended to benefit more from platinum chemotherapy than from platinum-free chemotherapy(P=0.05,P-interaction=0.02).Conclusions:HRD characterization may guide decision-making regarding the use of platinum treatment in patients with TNBC in both adjuvant and metastatic settings.

关键词： Homologous recombination deficiency triple-negative breast cancer platinum survival BRCA

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platinum-Induced Pseudo-Zn-Air Reaction Massively Increases the Electrochemical Capacity of Aqueous Zn/V_(5)O_(12)·6H_(2)O Batteries

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Energy & Environmental Materials 2021年第4期4卷 596-602页

作者： Gongzheng Yang Chengxin Wang State Key Laboratory of Optoelectronic Materials and Technologies School of Materials Science and EngineeringSun Yat-sen(Zhongshan)UniversityGuangzhou 510275China The Key Laboratory of Low-carbon Chemistry&Energy Conservation of Guangdong Province Sun Yat-sen(Zhongshan)UniversityGuangzhou 510275China

How to effectively improve Zn^(2+)-storage properties is now becoming an urgent issue in the development of high-energy-density aqueous zinc-ion batteries.Here,a new method is proposed to massively increase the electrochemical capacity of aqueous Zn/V_(5)O_(12)·6H_(2)Obatteries.By adding a small amount of platinum(Pt,1.5 wt.%)and keeping other factors constant,the V_(5)O_(12)·6H_(2)O-Pt electrodes deliver a much higher specific capacity(440 m Ah g^(-1)at 500 m A g^(-1))than do V_(5)O_(12)·6H_(2)Oelectrodes(270 m Ah g^(-1)at500 m A g^(-1)).The structural and morphological evolution of V_(5)O_(12)·6H_(2)Oduring cycling results in Zn^(2+)ion insertion/extraction and the formation/disappearance of the zinc hydroxyl complex(Zn_(4)SO_(4)(OH)_(6)·5H_(2)O,ZHS),where the latter is closely related to the surface redox reaction,promoting Zn^(2+)ion stripping/plating on the Zn anode and consequently leading to extra electron transfer.Electrochemical tests in the absence of oxygen reveal that the Pt additive has no contribution and is even counterproductive to electric conductivity but favors remarkable enhancement of the pseudocapacitance.Accordingly,it is apparent that a strong causal relationship exists between Pt and the ZHS.In consideration of the catalytic application for oxygen reduction,Pt is expected to play a vital role in enhancing the electrochemical capacity through the pseudo-Zn-air reaction.This finding introduces a new strategy for achieving high-performance aqueous zinc-ion batteries.

关键词： cathode platinum pseudo-Zn-air reaction V_(5)O_(12)·6H_(2)O Zinc-ion battery

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Genome-wide analysis identify novel germline genetic variations in ADCY1 influencing platinum-based chemotherapy response in nonsmall cell lung cancer

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Acta Pharmaceutica Sinica B 2022年第3期12卷 1514-1522页

作者： Chenxue Mao Juan Chen Ting Zou Yuankang Zhou Junyan Liu Xi Li Xiangping Li Min Li Pinhua Pan Wei Zhuo Yang Gao Shuo Hu Desheng Xiao Lin Wu Zhan Wang Heng Xu Wen Yang Yingjie Xu Haihua Xiao Kazuhiko Hanada Wei Zhang Honghao Zhou Jiye Yin Zhaoqian Liu Departments of Clinical Pharmacology and Pharmacy Hunan Key Laboratory of Pharmacogeneticsand National Clinical Research Center for Geriatric DisordersXiangya HospitalCentral South UniversityChangsha 410008China Institute of Clinical Pharmacology Engineering Research Center of Applied Technology of PharmacogenomicsMinistry of EducationCentral South UniversityChangsha 410078China Department of Respiratory Xiangya HospitalCentral South UniversityChangsha 410008China Department of Thoracic Surgery Xiangya HospitalCentral South UniversityChangsha 410008China Department of Nuclear Medicine Xiangya HospitalCentral South UniversityChangsha 410008China Department of Pathology Xiangya HospitalCentral South UniversityChangsha 410014China Department of Thoracic Medicine Hunan Cancer HospitalChangsha 410014China Department of Medical Oncology Lung Cancer and Gastrointestinal UnitHunan Cancer HospitalChengdu 610000China State Key Laboratory of Biotherapy and Cancer Center West China HospitalSichuan University and Collaborative Innovation Center of BiotherapyChengdu 610000China Department of Molecular and Cellular Biochemistry School of MedicineShanghai Jiaotong UniversityShanghai 200025China Beijing National Laboratory for Molecular Sciences State Key Laboratory of Polymer Physics and ChemistryInstitute of ChemistryChinese Academy of SciencesBeijing 100190China Department of Pharmacometrics and Pharmacokinetics Meiji Pharmaceutical University Tokyo 204-8588Japan

To explore the pharmacogenomic markers that affect the platinum-based chemotherapy response in non-small-cell lung carcinoma(NSCLC),we performed a two-cohort of genome-wide association studies(GWAS),including 34 for WES-based and 433 for microarray-based analyses,as well as two independent validation cohorts.After integrating the results of two studies,the genetic variations related to the platinum-based chemotherapy response were further determined by fine-mapping in 838 samples,and their potential functional impact were investigated by eQTL analysis and in vitro cell experiments.We found that a total of 68 variations were significant at Pplatinum-based chemotherapy.In conclusion,our study found that rs2280496 and rs189178649 in ADCY1 gene were associated the sensitivity of platinum-based chemotherapy in NSCLC patients.

关键词： Pharmacogenomics NSCLC platinum GWAS WES ADCY1 Precious medicine SNPs

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platinum drugs:from Pt(Ⅱ)compounds,Pt(Ⅳ)prodrugs,to Pt nanocrystals/nanoclusters

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Science Bulletin 2017年第8期62卷 589-596页

作者： Xi Hu Fangyuan Li Nabila Noor Daishun Ling Zhejiang Province Key Laboratory of Anti-Cancer Drug Research College of Pharrnaceutical SciencesZhejiang UniversityHangzhou 310058China Key Laboratory of Biomedical Engineering of the Ministry of Education College of Biomedical Engineering&Instrument ScienceZhejiang UniversityHangzhou 310027China

platinum(Pt) based drugs, such as cisplatin, are widely used as anti-cancer agents, but their severe adverse reactions and resistance of cancer patients have limited their board clinical use. For the last few decades, Pt(Ⅱ) compounds, Pt(Ⅳ) prodrugs as well as smart drug delivery systems have been developed to overcome these problems. However, most conventional strategies rely on the similar anti-cancer mechanism with cisplatin and consequently only achieve limited success. Recently, Pt nanocrystals/nanoclusters(Pt NCs), with a brand new anti-cancer mechanism, have shown a promising potential in targeted cancer therapy, especially in Pt resistance circumvention. This review is helpful to understand the research strategies of Pt drugs, particularly, the recent developments and medical applications of Pt NCs.

关键词： platinum Pt(Ⅱ) Pt(Ⅳ) Pt nanocrystals/nanoclusters Pt resistance Cancer therapy

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platinum Atoms Dispersed in Single-chain Polymer Nanoparticles

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Chinese Journal of Polymer Science 2021年第4期39卷 441-446,I0005页

作者： Zhi-Yu Hu Hong-Ting Pu Jian-Guo Wu Department of Polymeric Materials School of Materials Science&EngineeringTongji UniversityShanghai 201804China Key Laboratory of Advanced Civil Engineering Materials School of Materials Science&EngineeringTongji UniversityShanghai 201804China

The intramolecular cross-linking of single polymer chains can form single-chain nanoparticles(SCNPs),which have many applications.In this study,styrenic copolymers with pendent triphenylphosphine as the coordination site for platinum ions(Pt(Ⅱ))and benzocyclobutene as the latent reactive groups are synthesized.Triphenylphosphine groups in the chains can coordinate Pt(Ⅱ)and aid slight single-chain folding in dilute solution.The intramolecular cross-linking caused by the ring-open reaction of benzocyclobutene completes the single-chain collapse and forms stable SCNPs in dilute solution.Pt(Ⅱ)embedded in SCNPs can be further reduced to platinum atoms(Pt(0)).Pt(0)steadily and atomically dispersed in SCNPs exhibits better catalytic properties than normal polymer carried platinum particles do for the reduction of p-nitrophenol to p-aminophenol.

关键词： Single-chain Polymer nanoparticles Intramolecular cross-linking platinum Coordination

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Interfacial engineering of atomic platinum-doped molybdenum carbide quantum dots for high-rate and stable hydrogen evolution reaction in proton exchange membrane water electrolysis

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Nano Research 2023年第10期16卷 12186-12195页

作者： Lulu Chen Yichao Huang Yanping Ding Ping Yu Fang Huang Wenbo Zhou Limin Wang Yangyang Jiang Haitao Li Hanqing Cai Lin Wang Hang Wang Meihong Liao Lianming Zhao Zhuangjun Fan State Key Laboratory of Heavy Oil Processing School of Materials Science and EngineeringChina University of Petroleum(East China)Qingdao 266580China Shandong Saikesaisi Hydrogen Energy Co. LtdJinan 250013China School of Mechanical and Electronic Engineering Qingdao Binhai UniversityQingdao 266555China

platinum(Pt)-based electrocatalysts remain the only practical cathode catalysts for proton exchange membrane water electrolysis(PEMWE),due to their excellent catalytic activity for acidic hydrogen evolution reaction(HER),but are greatly limited by their low reserves and high cost.Here,we report an interfacial engineering strategy to obtain a promising low-Pt loading catalyst with atomically Pt-doped molybdenum carbide quantum dots decorated on conductive porous carbon(Pt-MoCx@C)for high-rate and stable HER in PEMWE.Benefiting from the strong interfacial interaction between Pt atoms and the ultra-small MoCx quantum dots substrate,the Pt-MoCx catalyst exhibits a high mass activity of 8.00 A·mgPt−1,5.6 times higher than that of commercial 20 wt.%Pt/C catalyst.Moreover,the strong interfacial coupling of Pt and MoCx substrate greatly improves the HER stability of the Pt-MoCx catalyst.Density functional theory studies further confirm the strong metal-support interaction on Pt-MoCx,the critical role of MoCx substrate in the stabilization of surface Pt atoms,as well as activation of MoCx substrate by Pt atoms for improving HER durability and activity.The optimized Pt-MoCx@C catalyst demonstrates>2000 h stability under a water-splitting current of 1000 mA·cm^(−2)when applied to the cathode of a PEM water electrolyzer,suggesting the potential for practical applications.

关键词： proton exchange membrane(PEM)water electrolysis hydrogen evolution reaction electrocatalysts molybdenum carbides platinum

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Synergy of first-and second-sphere interactions in a covalent organic framework boosts highly selective platinum uptake

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Science China Chemistry 2023年第3期66卷 783-790页

作者： Linwei He Baoyu Li Zhonglin Ma Lixi Chen Shicheng Gong Mingxing Zhang Yaoyao Bai Qi Guo Fuqi Wu Fuqiang Zhao Jie Li Duo Zhang Daopeng Sheng Xing Dai Long Chen Jie Shu Zhifang Chai Shuao Wang State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhou 215123China Analysis and Testing Center Soochow UniversitySuzhou 215123China

platinum recovery from waste electrical and electronic equipment(WEEE) in highly acidic solutions is significant to the electronics industry and environmental remediation. However, the lack of ingenious design and synergetic coordination gives rise to unsatisfied PtCl_(4)^(2-)extraction capacities and selectivities in most previously reported adsorbents(e.g., polymeric and inorganic materials). Herein, we proposed a synergistic strategy that realizes highly selective PtCl_(4)^(2-)uptake through first-and second-sphere coordinations. The proof-of-concept imine-linked covalent organic framework(SCU-COF-3) was found to chelate Pt Cl42-via the direct N…Pt coordination and the synergistically interlaminar N–H…Cl hydrogen bonds, which was disclosed by the comprehensive analysis of extended X-ray adsorption fine structure(EXAFS) characterizations and density functional theory(DFT) calculations. The unique adsorption mechanism imparts a superior adsorption capacity(168.4 mg g-1)and extraordinary Pt(II) selectivity to SCU-COF-3 under static conditions. In addition, SCU-COF-3 exhibits an upgraded distribution coefficient of 1.62 × 10^(5)mL· g^(-1), one order of magnitude higher than those of reported natural adsorbents. Specifically, SCU-COF-3 can extract PtCl_(4)^(2- )quantitatively from a simulated acidic waste solution coexisting with other 12 competitive ions, suggesting its promising application in practical scenarios.

关键词： covalent organic frameworks platinum hydrogen bond adsorption

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platinum in-situ catalytic oleylamine combustion removal process for carbon supported platinum nanoparticles

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Journal of Energy Chemistry 2020年第2期29卷 120-125页

作者： Qingying Zhao Huanqiao Li Xiaoming Zhang Shansheng Yu Suli Wang Gongquan Sun Division of Fuel Cells and Battery Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina2 University of Chinese Academy of Sciences Beijing 100049China Department of Materials Science Jilin UniversityChangchun 130012JilinChina

Colloidal synthesis method such as oleylamine(OAm)-stabilized process is of great interest for obtaining uniform and highly dispersed platinum nanoparticle catalysts, yet the ligand may unavoidably inhibit their electro-catalytic performance. Thus, fully removing these ligands is critical to activate catalyst surface. Previous research of OAm removal process pointed that thermal annealing was the most effective way in comparison with other methods such as chemical washing, UV–Ozone irradiation and cyclic voltammetry sweeping, but generally resulting in undesired growth of platinum nanoparticle. Few studies concerning a more efficient ligand removal process have been published yet. In this work we proposed a platinum in-situ catalytic OAm combustion strategy to elucidate the removal mechanism of OAm ligands in thermal process and the key experimental parameters were also optimized. In addition, heat flow signal based on differential scanning calorimetry(DSC) measurement as a sensitive indicator, is suggested to reveal the ligand removal efficiency, which is much more reliable than the traditional spectroscopy.In comparison with commercial Pt/C sample, such a surface clean Pt/C electrocatalyst has shown an enhanced specific activity for oxygen reduction reaction. Our removal strategy and the evaluation method are highly instructive to efficient removal of different organic ligands.

关键词： Ligand removal platinum in-situ catalytic OAm combustion Carbon supported platinum electro-catalyst ORR

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