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Covalently Bonded Ni Sites in Black Phosphorene with Electron Redistribution for Efficient Metal‑Lightweighted Water Electrolysis

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Nano-Micro Letters 2024年第6期16卷 233-245页

作者： Wenfang Zhai Ya Chen Yaoda Liu Yuanyuan Ma Paranthaman Vijayakumar Yuanbin Qin yongquan qu Zhengfei Dai State Key Laboratory for Mechanical Behavior of Materials Xi’an Jiaotong UniversityXi’an 710049People’s Republic of China School of Chemistry and Chemical Engineering Northwestern Polytechnical UniversityXi’an 710072People’s Republic of China SSN Research Centre SSN College of EngineeringChennaiTamil Nadu 603110India

The metal-lightweighted electrocatalysts for water splitting are highly desired for sustainable and economic hydrogen energy deployments,but *** this work,a low-content Ni-functionalized approach triggers the high capability of black phosphorene(BP)with hydrogen and oxygen evolution reaction(HER/OER)*** a facile in situ electro-exfoliation route,the ionized Ni sites are covalently functionalized in BP nanosheets with electron redistribution and controllable metal *** is found that the as-fabricated Ni-BP electrocatalysts can drive the water splitting with much enhanced HER and OER *** 1.0 M KOH electrolyte,the optimized 1.5 wt%Nifunctionalized BP nanosheets have readily achieved low overpotentials of 136 mV for HER and 230 mV for OER at 10 mA cm^(−2).Moreover,the covalently bonding between Ni and P has also strengthened the catalytic stability of the Ni-functionalized BP electrocatalyst,stably delivering the overall water splitting for 50 h at 20 mA cm^(−2).Theoretical calculations have revealed that Ni–P covalent binding can regulate the electronic structure and optimize the reaction energy barrier to improve the catalytic activity *** work confirms that Ni-functionalized BP is a suitable candidate for electrocatalytic overall water splitting,and provides effective strategies for constructing metal-lightweighted economic electrocatalysts.

关键词： Black phosphorus Water electrolysis Electrocatalyst Electron redistribution Covalent functionalization

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Describing Hadsorption on dual-active sites of single-atom-metals and frustrated-Lewis-pairs for reverse water-gas shift reaction

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Science China Chemistry 2024年

作者： Wenbin Li Jie Gan Qing Guo Sai Zhang yongquan qu School of Chemistry and Chemical Engineering Northwestern Polytechnical University School of Materials and Environmental Engineering Chizhou University Research & Development Institute of Northwestern Polytechnical University in Shenzhen

Acquiring descriptors to guide catalyst design is an ideal but challenging topic in the field of heterogeneous catalysis. Herein, the adsorption energy of H*(Ead（H）) has been established to describe the catalytic activity of dual-active sites of single-atom metals and frustrated Lewis pairs （FLPs） on the porous nanorod of CeO2surface （M1/PN-CeO2） for reverse water-gas shift （RWGS）reaction. H2and CO2molecules are adsorbed and activated on single-atom metals and FLP sites, respectively, facilitating the RWGS reaction through the H*spillover from single-atom metals to PN-CeO2supports. Mechanistic investigations illustrate that the generation of H*on the single-atom metals and subsequent migration towards FLP are critical steps, determining the performance of M1/PN–CeO2for RWGS reaction. A volcanic correlation is observed between Ead（H） and catalytic activity of M1/PN–CeO2for RWGS. The Pt1/PN–CeO2catalysts with a minimal deviation of-0.01 eV from the experimentally optimized Ead（H） of-1.88 eV, exhibited an exceptional turnover frequency of 33,605 h-1and surpassed a turnover number of 20,000,000for each Pt active site during a period of 650 h at 600°C. These findings could pave the way for the rational design of highly active and durable catalysts for RWGS reaction.

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Engineering the axial coordination of cobalt single atom catalysts for efficient photocatalytic hydrogen evolution

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Nano Research 2024年第6期17卷 5114-5121页

作者： Ning Kang Lingwen Liao Xue Zhang Zhen He Binlu Yu Jiahong Wang yongquan qu Paul KChu Seeram Ramakrishna Xue-Feng Yu Xin Wang Licheng Bai Materials Interfaces Center Shenzhen Institute of Advanced TechnologyChinese Academy of Sciences(CAS)Shenzhen 518055China Key Laboratory of Materials Physics Anhui Key Laboratory of Nanomaterials and NanotechnologyCAS Center for Excellence in NanoscienceInstitute of Solid State PhysicsChinese Academy of SciencesHefei 230031China Department of Chemistry City University of Hong KongKowloonHong Kong 999077China Hong Kong Branch of National Precious Metals Material Engineering Research Center(NPMM) City University of Hong KongKowloonHong Kong 999077China Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an 710072China Department of Physics and Department of Materials Science and Engineering City University of Hong KongKowloonHong Kong 999077China National University of Singapore(NUS)Centre for Nanofibers and Nanotechnology Department of Mechanical EngineeringNational University of SingaporeSingapore 117542Singapore

Improving the catalytic activity of non-noble metal single atom catalysts(SACs)has attracted considerable attention in materials *** optimizing the local electronic structure of single atom can greatly improve their catalytic activity,it often involves in-plane modulation and requires high ***,we report a novel strategy to manipulate the local electronic structure of SACs via the modulation of axial Co-S bond anchored onto graphitic carbon nitride(C_(3)N_(4))at room temperature(RT).Each Co atom is bonded to four N atoms and one S atom(Co-(N,S)/C_(3)N_(4)).Owing to the greater electronegativity of S in the Co-S bond,the local electronic structure of the Co atoms is available to be controlled at a relatively moderate ***,when employed for the photocatalytic hydrogen evolution reaction,the adsorption energy of intermediate hydrogen(H*)on the Co atoms is remarkably *** the presence of the Co-(N,S)/C_(3)N_(4)SACs,the hydrogen evolution rates reach up to 10 mmol/(g·h),which is nearly 10 and 2.5 times greater than the rates in the presence of previously reported transition metal/C_(3)N_(4)and noble platinum nanoparticles(PtNPs)/C_(3)N_(4)catalysts,*** to the tailorable axial Co-S bond in the SAC,the local electronic structure of the Co atoms can be further optimized for other photocatalytic *** axial coordination engineering strategy is universal in catalyst designing and can be used for a variety of photocatalytic applications.

关键词： transition metal single-atom local electronic structure photocatalytic hydrogen evolution graphitic carbon nitride axial coordination environment

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Sorafenib sensitization in tumor therapy by iron overload and AMPK activation

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Nano Research 2024年第7期17卷 6386-6399页

作者： Jun Zhu Shoujie Zhao Yejing Zhu Shouzheng Ma Tenghui Han Fenghua Xu Huichen Li Bo Wang Zhixiong Guo Da Chen yongquan qu Zhimin Tian Junlong Zhao Lei Liu State Key Laboratory of Holistic Integrative Management of Gastrointestinal Cancers National Clinical Research Center for Digestive DiseasesXijing HospitalFourth Military Medical UniversityXi’an 710032China Department of General Surgery The Southern Theater Air Force HospitalGuangzhou 510602China Department of General Surgery Tangdu HospitalFourth Military Medical UniversityXi’an 710038China Department of Thoracic Surgery Tangdu HospitalFourth Military Medical UniversityXi’an 710038China Department of Neurology Airborne Army HospitalWuhan 430012China Key Laboratory of Modern Teaching Technology(Ministry of Education) Shaanxi Normal UniversityXi’an 710062China State Key Laboratory of Holistic Integrative Management of Gastrointestinal Cancers Department of Biochemistry and Molecular BiologySchool of Basic MedicineFourth Military Medical UniversityXi’an 710032China Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an 710072China State Key Laboratory of Holistic Integrative Management of Gastrointestinal Cancers Department of Medical Genetics and Developmental BiologyFourth Military Medical UniversityXi’an 710032China Department of Pediatrics Tangdu HospitalFourth Military Medical UniversityXi’an 710000China

Sorafenib,as a first-line drug for advanced hepatocellular carcinoma(HCC),could trigger ferroptosis by inhibiting cystine/glutamate ***,low-level intracellular iron and insufficient activation of adenosine monophosphate(AMP)-activated protein kinase(AMPK)confer impaired response to *** this study,a unique sorafenib nanocomposite dexterously modified with Fe-Material of Institut Lavoisier(sora@Fe-MIL)was synthesized to escalate intracellular iron level and activate AMPK,further potentiating the ferroptotic effect of ***,this strategic deployment of sora@Fe-MIL triggered an extensive demise of cancer cells,while manifesting negligible deleterious impact on normal *** prominent ferroptosis biomarkers,glutathione peroxidase 4(GPX4)and solute carrier family 7 member 11(SLC7A11),underwent pronounced downregulation,underscoring the efficacy of this strategy in inducing ***,the bioactivity of AMPK was considerably elevated,and its downstream targets were conspicuously inhibited by the treatment with sora@*** orthotopic HCC animal models,we observed a substantial suppression of primary in situ tumor growth,and ribonucleic acid(RNA)sequencing elucidated an elevated degree of ferroptosis and AMPK activation with the treatment of sora@*** conclusion,we proposed that the meticulously designed strategy for secure and efficacious iron release and AMPK activation could significantly potentiate the ferroptotic impact of sorafenib,thus resuscitating its therapeutic response in HCC patients.

关键词： anti-tumor ferroptosis Fe-Material of Institut Lavoisier(Fe-MIL) sorafenib adenosine monophosphate(AMP)-activated protein kinase(AMPK)

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设计稳定的钌基析氢和析氧反应催化剂的基本原理

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Chinese Journal of Catalysis 2024年第5期60卷 68-106页

作者：苟王燕王译晨张铭凯谈晓荷马媛媛瞿永泉西北工业大学深圳研究院广东深圳518057 西北工业大学化学与化工学院陕西西安710072 西安理工大学理学院陕西西安710048

清洁和可再生能源具有地域性和间歇性,需要能量转换和存储技术来解决这些问题.氢气(H_(2))具有无毒、易得、经济、储量丰富和零碳排放的优势,作为能源媒介展现出巨大的潜力.而电分解水技术,因其高效性和便利性,成为了一种极具吸引力、... 详细信息

清洁和可再生能源具有地域性和间歇性,需要能量转换和存储技术来解决这些问题.氢气(H_(2))具有无毒、易得、经济、储量丰富和零碳排放的优势,作为能源媒介展现出巨大的潜力.而电分解水技术,因其高效性和便利性,成为了一种极具吸引力、应用前景广阔且可靠的能源技术.研究表明,在较宽的pH范围内,贵金属催化剂仍然是最优的析氢反应(HER)和析氧反应(OER)催化剂.其中,钌(Ru)作为一种相对便宜的铂族金属,显示出在HER中替代商业铂碳(Pt/C)催化剂以及在OER中替代铱(Ir)的潜力.然而,尽管在提高钌基催化剂的催化活性方面取得了很大进展,但其稳定性问题仍然是阻碍其实际应用的主要障碍.因此,迫切需要全面梳理和综述关于设计稳定钌基HER和OER催化剂的基本原理和最新进展,更好地理解钌基催化剂的催化机理,深入认识影响其稳定性的关键因素,以期为解决这一挑战提供有力的理论支持和实践指导.本文系统总结了钌基催化剂在电分解水反应中关于稳定性研究的最新进展.首先,简要介绍了钌基催化剂在HER/OER中的反应机理以及与之相关的理论计算、原位表征技术、稳定性测试手段和评价标准等方面的研究进展.接下来,详细探讨了钌基催化剂在HER/OER过程中的失活机制,包括载体腐蚀、奥斯特瓦尔德成熟、团聚、颗粒脱离、活性位点中毒、金属溶解、过度氧化和晶体结构坍塌等.基于以上对失活机制的认识,进一步归纳了提高钌基催化剂稳定性的设计策略和机制.在HER方面,从引入导电基底、构筑核壳结构、形成镶嵌结构、增强金属-载体相互作用、相转变工程以及调节中间体吸附和脱附行为等方面阐述了提高钌基催化剂稳定性的策略.对于OER过程,也总结了一系列提高钌基催化剂OER稳定性的策略,包括与铱杂化、构筑核壳结构、引入稳定的载体、化学掺杂、形成固溶体以及转变反应路径.在分析了各种策略的优缺点并提出改进方向后,还概述了钌基催化剂在全电解水以及器件中的研究现状.最后,指出了钌基催化剂稳定性研究所面临的挑战和未来的研究方向:(1)需要更贴近工业实际的稳定性测试策略和评价标准;(2)对失活机制的进一步研究;(3)原位技术的进一步发展和应用;(4)探索更多先进的改性策略,如非晶态载体、范德华异质结、自旋态调节以及微环境调节等;(5)关注实际应用中可能遇到的问题,如催化剂大规模制备、双功能催化剂的设计以及杂质的影响.综上,本文系统地总结了钌基催化剂的反应机制、稳定性测试方法与评价标准、失活机制、设计策略、研究进展、具体应用以及目前存在的挑战,希望能够进一步促进该领域深入水平研究.同时,本文对光催化、热催化、酶催化等催化领域的研究也提供一定的参考和借鉴.

关键词：电催化水分解失活机理钌基催化剂稳定性

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Insights on catalytic mechanism of CeO2 as multiple nanozymes

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Nano Research 2022年第12期15卷 10328-10342页

作者： Yuanyuan Ma Zhimin Tian Wenfang Zhai yongquan qu Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an710072China

CeO2 with the reversible Ce3+/Ce4+redox pair exhibits multiple enzyme-like catalytic performance,which has been recognized as a promising nanozyme with potentials for disease diagnosis and *** surface physicochemical properties of various CeO2 catalysts with controllable sizes,morphologies,and surface states enable a rich surface chemistry for their interactions with various molecules and species,thus delivering a wide variety of catalytic behaviors under different *** the significant progress made in developing CeO2-based nanozymes and their explorations for practical applications,their catalytic activity and specificity are still uncompetitive to their counterparts of natural enzymes under physiological *** the attempt to provide the insights on the rational design of highly performed CeO2 nanozymes,this review focuses on the recent explorations on the catalytic mechanisms of CeO2 with multiple enzyme-like *** the detailed discussion and proposed perspectives,we hope this review can raise more interest and stimulate more efforts on this multi-disciplinary field.

关键词： heterogeneous catalysis ceria nanozyme oxygen vacancy

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Protection strategy for improved catalytic stability of silicon photoanodes for water oxidation

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Science Bulletin 2015年第16期60卷 1395-1402页

作者： Zhaoming Xia Xuemei Zhou Jing Li yongquan qu Center for Applied Chemical Research Frontier Institute of Science and Technology State Key Laboratory for Mechanical Behavior of Materials Xi’an Jiaotong University Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed Matter Ministry of Education Xi’an Jiaotong University

Silicon-based electrodes have attracted great attention in the artificial photosynthetic systems that mimic natural photosynthesis and directly convert the solar energy into chemical energy. Despite significant efforts to date,catalytic stability of the silicon photoelectrodes is limited by their poor electrochemical stability. The formation of passivation or protective layers provides a feasible strategy to improve the photocatalytic stability of silicon photoelectrodes. Many candidates including metals, metal oxides, metal silicides and polymers have been explored as the protection layers for silicon photoelectrodes. The present review gives a concise overview of the protected silicon photoanodes for water oxidation with a focus on the relationship between the structural architecture of silicon photoanodes and their photocatalytic activity and stability.

关键词： Silicon photoanode Photocatalysis Stability - Protection layer Water oxidation

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Single crystalline CeO_(2) nanotubes

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Nano Research 2021年第3期14卷 715-719页

作者： Fangxian Cao Mingkai Zhang Kaili Yang Zhimin Tian Jing Li yongquan qu Frontier Institute of Science and Technology Xi’an Jiaotong UniversityXi’an710049China College of Chemistry and Chemical Engineering Liaocheng UniversityLiaocheng252059China Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an710072China

Here,we report a facile synthetic methodology to prepare uniform single crystalline CeO_(2) nanotubes through a hydrothermal transformation of CeO_(2) nanorods in aqueous Ce(NO3)3 solution.A chemically driven etching-dissolution-deposition mechanism is proposed,involving the surface Ce^(3+)hydrolysis and dissolution at tips of nanorods and subsequent redeposition and crystallization on the outer sides of *** to CeO_(2) nanorods,CeO_(2) nanotubes exhibited the richer structural defects,higher reducibility and larger surface area,leading to a higher haloperoxidase-like activity.

关键词： CeO_(2)nanorod hydrothemal transformation CeO_(2)nanotube etching-dissolution-deposition mechanism haloperoxidase-like activity

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quaternary pyrite-structured nickel/cobalt phosphosulfide nanowires on carbon cloth as efficient and robust electrodes for water electrolysis

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Nano Research 2017年第3期10卷 814-825页

作者： Jiayuan Li Zhaoming Xia Xuemei Zhou Yuanbin Qin Yuanyuan Ma yongquan qu Center for Applied Chemical Research Frontier Institute of Science and Technology and State Key Laboratory for MechanicalBehavior of Materials Xi'an Jiaotong University Xi'an 710049 China

The strategy of element substitution is an effective way to tune the electronic structures of the active sites in catalysts, thereby leading to improvements in both the catalytic activity and stability. Herein, we design and synthesize pyrite-type nickel/phosphorus co-doped CoS2 nanowires on carbon cloth （NiCoPS/CC） as efficient and durable electrodes for water electrolysis. Introduction of nickel and phosphorus produced stepwise and superb enhancement of the performance of the electrodes in the hydrogen evolution reaction due to regulation of the electronic structures of the active sites of the catalyst and accelerated charge transfer over a wide pH range （0-14）. The NiCoPS/CC electrodes also delivered a nearly undecayed catalytic current density of 10 ***-2 at a low overpotential of 230 mV for oxygen evolution due to in situ formation of surficial Ni-Co oxo/hydroxide in 1.0 M KOH. Thus, the NiCoPS/CC electrodes gave rise to a catalytic current density of 10 mA·cm-2 for overall water splitting at potentials as low as 1.54 V during operation over 100 h in 1.0 M KOH with a Faradic efficiency of ~100%.

关键词： water electrolysis pyrite heterogeneous catalysis nanowire

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In-situ reconstruction of single-atom Pt on Co_(3)O_(4)for hydrogenation

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Nano Research 2023年第5期16卷 6507-6511页

作者： Sai Zhang Zhaoming Xia Wenbin Li You Wang Yong Zou Mingkai Zhang Zhongmiao Gong Yi Cui yongquan qu Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an 710072China Research&Development Institute of Northwestern Polytechnical University in Shenzhen Shenzhen 518057China Department of Chemistry Tsinghua UniversityBeijing 100084China Vacuum Interconnected Nanotech Workstation Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123China

Actual chemical states of single-atom metal on reducible supports remain a fiercely debated topic under reactive ***,we demonstrate that the single-atom Pt on Co_(3)O_(4)surface undergoes an in-situ reconstruction to form isolated Pt-Co bimetallic sites via reducing coordination number of Pt–O in the presence of hydrogen from both simulations and in-situ X-ray photoelectron *** modified chemical states of Pt greatly promoted H_(2)activation,thus delivering a significantly high turnover frequency of 7,448 h−1(19.5 times over Pt nanoparticles on Co_(3)O_(4))for hydrogenation of *** satisfactory selectivity of 95.2%towards cinnamyl alcohol was ascribed to a tilted adsorption configuration of reactant on the catalyst surface via aldehyde *** anticipate that the recognitions on in-situ reconstruction of single-atom catalysts(SACs)under the reducing conditions benefit the design of highly-performed hydrogenation catalysts.

关键词： single-atom catalysis(SACs) coordination environment Pt-Co bimetallic sites hydrogenation

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