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Nano Research 2024年第5期17卷 3879-3887页

作者： Yuting Chen Tian Meng Zhicai Xing Yueying Yan Yang Yang Bohan Yao Dewen Wang Xiurong Yang State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied Chemistry and engineering University of Science and Technology of ChinaHefei 230026China

Developing efficient pH-universal hydrogen evolution reaction(HER)catalysts is critical in the field of water electrolysis,however,which is severely hampered by the sluggish kinetics in alkaline ***,a ruthenium(Ru)incorporation induced vacancy engineering strategy is firstly proposed to precisely construct oxygen vacancy(V_(O))-riched cobalt-ruthenium metaphosphate(CRPO)for high-efficiency pH-universal *** V_(O) modifies the electronic structure,improves the superficial hydrophilic and gas spillover capacity,it also reduces the coordination number of Ru atoms and regulates the coordination *** calculations indicate that Ru tends to adsorb H_(2)O and H^(*),whereas V_(O) tends to adsorb OH^(-),which greatly promotes the H_(2)O adsorption and the dissociation of HO-H ***,CRPO-2 exhibits remarkable HER performance,the mass activity is about 18.34,21.73,and 38.07 times higher than that of Pt/C in acidic,neutral,and alkaline media,respectively,at the same time maintain excellent *** findings may pave a new avenue for the rational design of electrocatalysts toward pH-universal water electrolysis.

关键词： cobalt metaphosphate pH-universal hydrogen evolution reaction(HER) vacancy engineering low-coordination atoms oxygen vacancy

Recent advances in vacancy engineering for reliable lithiumsulfur batteries

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Rare Metals 2024年第2期43卷 455-477页

作者： Wen-Dong Liu Xiao Tang Jun-An Feng Chao-Yue Zhang Hao Liu Chuan Shi Xiao-Xian Zhao Jian-Jun Song College of Physics School of Chemistry and Chemical EngineeringQingdao UniversityQingdao266071China Faculty of Science Centre for Clean Energy TechnologySchool of Mathematical and Physical SciencesUniversity of Technology SydneySydneyNSW2007Australia Department of Chemistry College of ScienceHebei Agricultural UniversityBaoding071001China

The high-energy-density and low-cost features endow lithium-sulfur batteries with broad application ***,many drawbacks,especially the detrimental shuttle effect,have hindered the further development of *** response,a lot of new structures have been applied to suppress the shuttle effect and promote the development of ***,vacancy engineering has gained the attention of researchers due to its unique electronic *** review aims to analyze the application of vacancy engineering in ***,the electrochemistry of LSBs has been systematically discussed and the existing challenges as well as improvement tactics of LSBs have also been ***,the preparation methods and characterization technologies of various vacancies are summarized,including oxygen vacancies,sulfur vacancies,selenium vacancies,other anion vacancies,cation vacancies,*** latest applications of vacancy engineering in LSBs are also summarized in this ***,some prospects and insights for further investigation and practical application of vacancy engineering in LSBs are put forward.

关键词： Lithium-sulfur batteries(LSBs) Defects vacancy engineering Electronic structure Shuttle effect

vacancy engineering of oxidized Nb_(2)CTx MXenes for a biased nitrogen fixation

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Green Energy & Environment 2023年第4期8卷 1185-1194页

作者： Mengzhao Zhang Hanqing Yin Fuhao Jin Jingquan Liu Xuqiang Ji Aijun Du Wenrong Yang Zhen Liu College of Materials Science and engineering Institute for Graphene Applied Technology InnovationQingdao University308 Ningxia RoadQingdao266071China School of Chemistry and Physics and Centre for Materials Science Queensland University of TechnologyGardens Point CampusBrisbane4001Australia School of Life and Environmental Sciences Deakin University75 Pigdons RoadGeelongVIC 3216Australia

The artificial nitrogen(N_(2)) reduction reaction(NRR) via electrocatalysis is a newly developed methodology to produce ammonia(NH3) at ambient conditions,but faces the challenges in N_(2)activation and poor reaction ***,Nb-based MXenes are developed to remarkably enhance the NRR activity through the engineering of the stretched 3D structure and oxygen vacancies(VO).The theoretical studies indicate that N_(2)could be initially adsorbed on VOwith an end-on configuration,and the potential determining step might be the first hydrogenation *** catalysts achieve an NH3production rate of 29.1 μg h^(-1)mg_(cat)^(-1)and excellent Faradic efficiency of 11.5%,surpassing other Nbbased *** selectivity of NRR is assigned to the unique structure of the catalysts,including(1) the layered graphitic structure for fast electron transfer and active site distribution,(2) the reactive VOfor N_(2)adsorption and activation,and(3) the expanded interlayer space for mass transfer.

关键词： Nitrogen reduction reaction Nb-based MXenes Oxygen vacancy vacancy engineering Electrocatalysis

Pt/TiO_(2–x) nanofibrous aerogel for effective nitrogen reduction: A simple strategy for simultaneous Pt formation and TiO_(2–x) vacancy engineering

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Chinese Chemical Letters 2022年第2期33卷 1001-1005页

作者： Meng Zhang Jin Dai Shengmei Huang Dan Fang Yitao Liu Jianyong Yu Bin Ding Andreas Greiner Innovation Center for Textile Science and Technology College of TextilesDonghua UniversityShanghai 201620China Macromolecular Chemistry and Bavarian Polymer Institute University of BayreuthBayreuth 95440Germany

Electrocatalysis plays an increasingly important role in converting atmospheric molecules(e.g.,N_(2),CO_(2) and H_(2)O)to value-added products(e.g.,NH_(3),C_(2)H_(4)and H_(2)).However,developing a simple strategy for preparing catalysts with high performance for the effective conversion of clean energy is still full of ***,we describe a straightforward,one-step reduction method to achieve the formation of Pt nanoparticles(NPs)and the vacancy engineering of TiO_(2-x)nanofibers(NFs)simultaneously,which can be accomplished in 5 ***,a Pt/TiO_(2-x)nanofibrous aerogel(NA)with an ordered cellular archi-tecture is prepared through a directional freezing *** Pt/TiO_(2-x)NA with excellent mechanical properties can be made into a self-supporting electrode for electrocatalytic N_(2)reduction reaction(NRR),showing high NH_(3) yield rate(4.81×10^(-10)mol/s cm^(-2))and Faraday efficiency(14.9%)at-0.35 V ***.

关键词： vacancy engineering Pt nanoparticles TiO_(2–x)nanofibers Nanofibrous aerogel Electrocatalysis Nitrogen reduction

vacancy-engineering-mediated activation of excitonic transition for boosting visible-light-driven photocatalytic oxidative coupling of amines

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Nano Research 2023年第11期16卷 12655-12661页

作者： Wenxiu Liu Lei Li Peng Zhang Manqin Guan Ming Zuo Yinhua Zhao Hui Wang Xiaodong Zhang Yi Xie Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China Institute of Energy Hefei Comprehensive National Science CenterHefei 230031China

The light absorption properties of semiconductor-based photocatalysts to a large extent determine the relevant catalytic *** strategies in broadening the light absorption range are usually accompanied with unfavorable changes in redox ability and dynamics of photoinduced species that would confuse the comprehensive *** this work,we propose a nontrivial excitonic transition regulation strategy for gaining sub-bandgap light absorption in low-dimensional semiconductor-based *** bismuth oxybromide(BiOBr)as a model system,we highlight that the light absorption cut-off edge could be effectively extended up to 500 nm by introducing Bi *** the basis of theoretical simulations and spectroscopic analyses,we attributed the broadening of light absorption to the promotion of excitonic transition that is generally forbidden in pristine BiOBr system,associated with Bi-vacancy-induced excited-state symmetry *** addition,Bi vacancy was demonstrated to implement negligible effects on other photoexcitation properties like excited-state energy-level profiles and *** from these features,the defective sample exhibits a notable advantage in gaining visible-light-driven photocatalytic reactions.

关键词： semiconductor-based photocatalysts light absorption vacancy engineering excitonic transition selective oxidation

Tungsten Blue Oxide as a Reusable Electrocatalyst for Acidic Water Oxidation by Plasma-Induced vacancy engineering

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CCS Chemistry 2021年第3期3卷 1553-1561页

作者： Hanfeng Liang Zhen Cao Chuan Xia Fangwang Ming Wenli Zhang Abdul-Hamid Emwas Luigi Cavallo Husam N.Alshareef Materials Science and engineering Physical Science and Engineering DivisionKing Abdullah University of Science and Technology(KAUST)Thuwal 23955 KAUST Catalysis Center(KCC) King Abdullah University of Science and Technology(KAUST)Thuwal 23955 Department of Chemical and Biomolecular engineering Rice UniversityHoustonTX 770054 Core LabsKing Abdullah University of Science and Technology(KAUST)Thuwal 23955 Core Labs King Abdullah University of Science and Technology(KAUST)Thuwal 23955

In contrast to alkaline water electrolysis,acidic water electrolysis remains an elusive goal due to the lack of earth-abundant,efficient,and acid-stable water oxidation ***,we show that materials with intrinsically poor electrocatalytic activity can be turned into active electrocatalysts that drive the acidic oxygen evolution reaction(OER)*** development is achieved through ultrafast plasma sputtering,which introduces abundant oxygen vacancies that reconstruct the surface electronic structures,and thus,regulated the surface interactions of electrocatalysts and the OER *** tungsten oxide(WO_(3))as an example,we present a broad spectrum of theoretical and experimental characterizations that show an improved energetics of OER originating from surface oxygen vacancies and resulting in a significantly boosted OER performance,compared with pristine WO_(3).Our result suggests the efficacy of using defect chemistry to modify electronic properties and hence to improve the OER performance of known materials with poor activity,providing a new direction for the discovery of acid-stable OER catalysts.

关键词： WO_(3) vacancy engineering plasma acidic OER reusable electrocatalyst

Cu_(1.8)S基合金的热电性能和电稳定性增强:熵工程和Cu空位工程

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Science China Materials 2023年第5期66卷 2051-2060页

作者：周炜李和章单帜航张瑞卢士阔裴俊葛振华周敏王愿兵张波萍 Beijing Municipal Key Laboratory of New Energy Materials and Technologies School of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing 100083China National Institute for Materials Science(NIMS) Tsukuba 3050047Japan Faculty of Materials Science and engineering Kunming University of Science and technologyKunming 650093China Key Laboratory of Cryogenics Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China Wuhan Joule Yacht Science&Technology Co. Ltd.Wuhan 430070China

无污染、低成本和高性能Cu_(1.8)S基类液态热电材料受到关注.但是,其过高的本征Cu空位和Cu离子迁移特性限制了其性能和电稳定性的进一步提升.本研究采用机械合金化结合放电等离子体烧结制备了一系列Cu_(1.8)S和Mn_(x)Cu_(1.8)S_(0.5)Se_... 详细信息

无污染、低成本和高性能Cu_(1.8)S基类液态热电材料受到关注.但是,其过高的本征Cu空位和Cu离子迁移特性限制了其性能和电稳定性的进一步提升.本研究采用机械合金化结合放电等离子体烧结制备了一系列Cu_(1.8)S和Mn_(x)Cu_(1.8)S_(0.5)Se_(0.5)(0.01≤x≤0.06)块体热电材料.随着Se和Mn的引入,体系由低熵Cu_(1.8)S(0.4R^(*))转变为中熵MnxCu_(1.8)S_(0.5)Se_(0.5)(1.2R^(*)).构型熵的增加不仅提高了体系的结构对称性,MnxCu_(1.8)S_(0.5)Se_(0.5)室温下呈立方相结构,还增大了Mn的固溶度.高浓度Mn固溶有效填补了过高的本征Cu空位,降低了载流子浓度,优化了能带结构,提升了电输运性能.熵工程一方面增大了Cu离子迁移势垒,抑制Cu离子迁移.750 K下,即使电流密度达到24 A cm^(-2),Mn_(0.03)Cu_(1.8)S_(0.5)Se_(0.5)的电阻也几乎没有变化,显示出优异的电稳定性;同时可降低声速,软化晶格,降低晶格热导率.Mn_(0.06)Cu_(1.8)S_(0.5)Se_(0.5)的块体样品在773 K时获得最大ZT值0.79,相较于初始样品提高了两倍.结果表明熵工程结合Cu空位工程是提升Cu_(1.8)S基热电材料性能的有效策略.

关键词： Cu_(1.8)S thermoelectric entropy engineering vacancy engineering solid solubility

Sulfur-deficient Bi_(2)S_(3-x) synergistically coupling Ti_(3)C_(2)T_(x)-MXene for boosting electrocatalytic N_(2) reduction

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Nano Research 2022年第5期15卷 3991-3999页

作者： Yaojing Luo Peng Shen Xingchuan Li Yali Guo Ke Chu School of Materials Science and engineering Lanzhou Jiaotong UniversityLanzhou 730070China

Electrocatalytic nitrogen reduction reaction(NRR)is an appealing route for the sustainable NH_(3)synthesis,while developing efficientand durable NRR catalysts remains at the heart of achieving high-efficiency N_(2)-to-NH_(3)***,we rationally combine vacancy and interface engineering to design sulfur-deficient Bi2S3 nanoparticles decorated Ti_(3)C_(2)T_(x)-MXene as an effective NRR *** developed Bi2S3 nanoparticles decorated Ti_(3)C_(2)T_(x)-MXene(Bi2S3-xTi_(3)C_(2)T_(x))naturally contained abundant S-vacancies and exhibited a dramatically boosted NRR activity with an NH_(3)yield of 68.3μg·h^(-1)mg^(-1)(-0.6 V)and a Faradaic efficiency of 22.5%(-0.4 V),far superior to pure Bi_(2)S_(3)and Ti_(3)C_(2)T_(x)and surpassing almost all ever reported Bi-and MXene-based NRR *** investigations unveiled that the exceptional NRR activity of Bi_(2)S_(3-x)/Ti_(3)C_(2)T_(x)stemmed from its dual-active-center system involving both S-vacancies and interfacial-Bi sites,which could synergistically promote N_(2)adsorption and*N_(2)H formation to result in an energetic-favorable NRR process.

关键词： electrocatalytic nitrogen reduction bismuth catalyst MXene vacancy engineering interface engineering

缺陷辅助高阴离子S/Se/P掺杂助力高性能钠离子电容器的快速传荷动力学

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Science Bulletin 2021年第18期66卷 1858-1868,M0003页

作者：邓杏兰邹康宇 Roya Momen 蔡鹏陈军侯红帅邹国强纪效波 College of Chemistry and Chemical engineering Central South UniversityChangsha 410083China State Key Laboratory of Powder Metallurgy College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China School of Materials Science and engineering Zhengzhou UniversityZhengzhou 450002China

设计具有快速传荷动力学的二氧化钛负极材料是进一步构建高能量功率密度混合离子电容器的关键所在.本文提出一个氧空位辅助二氧化钛高阴离子掺杂的策略,合成了高含量硫/硒/磷掺杂的二氧化钛负极材料.通过实验结果与理论计算相结合,本文... 详细信息

设计具有快速传荷动力学的二氧化钛负极材料是进一步构建高能量功率密度混合离子电容器的关键所在.本文提出一个氧空位辅助二氧化钛高阴离子掺杂的策略,合成了高含量硫/硒/磷掺杂的二氧化钛负极材料.通过实验结果与理论计算相结合,本文系统地研究了氧空位辅助掺杂的可行性、硫掺杂对二氧化钛的影响以及二氧化钛负极材料倍率性能极大提升的深层次机理.研究发现,氧空位的引入可以使硫掺杂过程自发进行,高含量的硫掺杂在二氧化钛能带结构中引入S 2p,使得其能带间隙变小,导电率显著提升;同时,硫进入晶格后,离子的迁移能垒降低,离子迁移速率增加,传荷动力学提高.这项工作为实现阴离子的高含量掺杂和提升二氧化钛的电荷转移动力学提供了一种新的策略,为设计具有快速动力学的电极材料提供了行之有效的方法.

关键词： vacancy engineering Anion doping Charge transfer kinetics Sodium ion capacitors Titanium dioxide

Emerging Bismuth-Based Step-Scheme Heterojunction Photocatalysts for Energy and Environmental Applications

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Renewables 2023年第5期1卷 485-513页

作者： Diejing Feng Xinyu Li Yanping Liu Xiaobo Chen Shijie Li National engineering Research Center for Marine Aquaculture Key Laboratory of Health Risk Factors for Seafood of Zhejiang ProvinceInstitute of Innovation&ApplicationZhejiang Ocean UniversityZhoushanZhejiang 316022 Department of Chemistry University of Missouri–Kansas CityKansas CityMissouri 64110

Photocatalysis has been expected to be a promising advanced oxidation process to endlessly convert exhaustless solar energy into storable,transportable,and usable chemical *** a kind of visible light-response semiconductors,Bi-based semiconductors can be developed into step-scheme(S-scheme)heterojunction photocatalysts,consisting of a reductive photocatalyst(RP)and an oxidative photocatalyst(OP)with band edge *** review sums up the state-of-the-art progress in Bi-based S-scheme heterojunctions,as well as the in-/ex-situ experiments and theoretical calculations to uncover the unique heterostructure and charge transfer mechanism of Bi-based S-scheme heterojunctions in *** can find that Bi-based S-scheme heterojunction photocatalysts have advantages in impeding the recombination of photo-induced electron-hole pairs,expediting the charge transfer,broadening solar energy utilization,and maximizing the potential energy of photo-redox reaction ***,the recently published work on the potential applications of Bi-based S-scheme heterojunctions is also summarized,including photocatalytic H_(2) production,CO_(2) reduction with water,pollutant degradation,H_(2)O_(2) production,and N_(2) photofixation for ammonia and urea production by comparing and discussing their photocatalytic *** the basis of research progress,the immediate challenges and future perspectives of Bi-based S-scheme heterojunction photocatalysts are critically debated.

关键词： Bismuth-based(Bi-based)semiconductors S-scheme heterojunction internal electric field Fermi level photocatalysis vacancy engineering