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Vivent les vacances!
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《法语学习》 2010年第3期23-23,45,共2页
Savez-vous que chaque été,des millions de Franais partent en vacances ? En effet,tous les Franais attendent impatiemment les vacances après une longue année de dur travail.Si certains vont ... Savez-vous que chaque été,des millions de Franais partent en vacances ? En effet,tous les Franais attendent impatiemment les vacances après une longue année de dur travail.Si certains vont à la mer,d'autres se reposent à la campagne ou visitent un pays étranger. 展开更多
关键词 Vivent les vacances SI
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High-efficiency sodium storage of Co_(0.85)Se/WSe_(2) encapsulated in N-doped carbon polyhedron via vacancy and heterojunction engineering 被引量:3
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作者 Ya Ru Pei Hong Yu Zhou +5 位作者 Ming Zhao Jian Chen Li Xin Ge Wei Zhang Chun Cheng Yang Qing Jiang 《Carbon Energy》 SCIE EI CAS CSCD 2024年第1期94-107,共14页
With the advantage of fast charge transfer,heterojunction engineering is identified as a viable method to reinforce the anodes'sodium storage performance.Also,vacancies can effectively strengthen the Na+adsorption... With the advantage of fast charge transfer,heterojunction engineering is identified as a viable method to reinforce the anodes'sodium storage performance.Also,vacancies can effectively strengthen the Na+adsorption ability and provide extra active sites for Na+adsorption.However,their synchronous engineering is rarely reported.Herein,a hybrid of Co_(0.85)Se/WSe_(2) heterostructure with Se vacancies and N-doped carbon polyhedron(CoWSe/NCP)has been fabricated for the first time via a hydrothermal and subsequent selenization strategy.Spherical aberration-corrected transmission electron microscopy confirms the phase interface of the Co_(0.85)Se/WSe_(2) heterostructure and the existence of Se vacancies.Density functional theory simulations reveal the accelerated charge transfer and enhanced Na+adsorption ability,which are contributed by the Co_(0.85)Se/WSe_(2) heterostructure and Se vacancies,respectively.As expected,the CoWSe/NCP anode in sodium-ion battery achieves outstanding rate capability(339.6 mAh g^(−1) at 20 A g^(−1)),outperforming almost all Co/W-based selenides. 展开更多
关键词 Co_(0.85)Se/WSe_(2)heterostructure density functional theory simulations N-doped carbon polyhedron Se vacancies sodium-ion batteries
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Boosting Hydrogen Storage Performance of MgH_(2) by Oxygen Vacancy-Rich H-V_(2)O_(5) Nanosheet as an Excited H-Pump 被引量:2
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作者 Li Ren Yinghui Li +4 位作者 Zi Li Xi Lin Chong Lu Wenjiang Ding Jianxin Zou 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第8期398-416,共19页
MgH_(2) is a promising high-capacity solid-state hydrogen storage material,while its application is greatly hindered by the high desorption temperature and sluggish kinetics.Herein,intertwined 2D oxygen vacancy-rich V... MgH_(2) is a promising high-capacity solid-state hydrogen storage material,while its application is greatly hindered by the high desorption temperature and sluggish kinetics.Herein,intertwined 2D oxygen vacancy-rich V_(2)O_(5) nanosheets(H-V_(2)O_(5))are specifically designed and used as catalysts to improve the hydrogen storage properties of MgH_(2).The as-prepared MgH_(2)-H-V_(2)O_(5) composites exhibit low desorption temperatures(Tonset=185℃)with a hydrogen capacity of 6.54 wt%,fast kinetics(Ea=84.55±1.37 kJ mol^(-1) H_(2) for desorption),and long cycling stability.Impressively,hydrogen absorption can be achieved at a temperature as low as 30℃ with a capacity of 2.38 wt%within 60 min.Moreover,the composites maintain a capacity retention rate of~99%after 100 cycles at 275℃.Experimental studies and theoretical calculations demonstrate that the in-situ formed VH_(2)/V catalysts,unique 2D structure of H-V_(2)O_(5) nanosheets,and abundant oxygen vacancies positively contribute to the improved hydrogen sorption properties.Notably,the existence of oxygen vacancies plays a double role,which could not only directly accelerate the hydrogen ab/de-sorption rate of MgH_(2),but also indirectly affect the activity of the catalytic phase VH_(2)/V,thereby further boosting the hydrogen storage performance of MgH_(2).This work highlights an oxygen vacancy excited“hydrogen pump”effect of VH_(2)/V on the hydrogen sorption of Mg/MgH_(2).The strategy developed here may pave a new way toward the development of oxygen vacancy-rich transition metal oxides catalyzed hydride systems. 展开更多
关键词 Hydrogen storage MgH_(2) V_(2)O_(5)nanosheets Oxygen vacancies VH_(2)
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Co/CoO heterojunction rich in oxygen vacancies introduced by O_(2) plasma embedded in mesoporous walls of carbon nanoboxes covered with carbon nanotubes for rechargeable zinc-air battery 被引量:2
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作者 Leijun Ye Weiheng Chen +1 位作者 Zhong-Jie Jiang Zhongqing Jiang 《Carbon Energy》 SCIE EI CAS CSCD 2024年第7期14-25,共12页
Herein,Co/CoO heterojunction nanoparticles(NPs)rich in oxygen vacancies embedded in mesoporous walls of nitrogen-doped hollow carbon nanoboxes coupled with nitrogen-doped carbon nanotubes(P-Co/CoOV@NHCNB@NCNT)are well... Herein,Co/CoO heterojunction nanoparticles(NPs)rich in oxygen vacancies embedded in mesoporous walls of nitrogen-doped hollow carbon nanoboxes coupled with nitrogen-doped carbon nanotubes(P-Co/CoOV@NHCNB@NCNT)are well designed through zeolite-imidazole framework(ZIF-67)carbonization,chemical vapor deposition,and O_(2) plasma treatment.As a result,the threedimensional NHCNBs coupled with NCNTs and unique heterojunction with rich oxygen vacancies reduce the charge transport resistance and accelerate the catalytic reaction rate of the P-Co/CoOV@NHCNB@NCNT,and they display exceedingly good electrocatalytic performance for oxygen reduction reaction(ORR,halfwave potential[EORR,1/2=0.855 V vs.reversible hydrogen electrode])and oxygen evolution reaction(OER,overpotential(η_(OER,10)=377mV@10mA cm^(−2)),which exceeds that of the commercial Pt/C+RuO_(2) and most of the formerly reported electrocatalysts.Impressively,both the aqueous and flexible foldable all-solid-state rechargeable zinc-air batteries(ZABs)assembled with the P-Co/CoOV@NHCNB@NCNT catalyst reveal a large maximum power density and outstanding long-term cycling stability.First-principles density functional theory calculations show that the formation of heterojunctions and oxygen vacancies enhances conductivity,reduces reaction energy barriers,and accelerates reaction kinetics rates.This work opens up a new avenue for the facile construction of highly active,structurally stable,and cost-effective bifunctional catalysts for ZABs. 展开更多
关键词 HETEROJUNCTION oxygen evolution/reduction reaction oxygen vacancies rechargeable zinc–air battery three‐dimensional nitrogen‐doped hollow carbon nanoboxes
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Impact of Transition Metal Layer Vacancy on the Structure and Performance of P2 Type Layered Sodium Cathode Material 被引量:1
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作者 Orynbay Zhanadilov Sourav Baiju +7 位作者 Natalia Voronina Jun Ho Yu A.-Yeon Kim Hun‑Gi Jung Kyuwook Ihm Olivier Guillon Payam Kaghazchi Seung‑Taek Myung 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第11期340-358,共19页
This study explores the impact of introducing vacancy in the transition metal layer of rationally designed Na_(0.6)[Ni_(0.3)Ru_(0.3)Mn_(0.4)]O_(2)(NRM)cathode material.The incorporation of Ru,Ni,and vacancy enhances t... This study explores the impact of introducing vacancy in the transition metal layer of rationally designed Na_(0.6)[Ni_(0.3)Ru_(0.3)Mn_(0.4)]O_(2)(NRM)cathode material.The incorporation of Ru,Ni,and vacancy enhances the structural stability during extensive cycling,increases the operation voltage,and induces a capacity increase while also activating oxygen redox,respectively,in Na_(0.7)[Ni_(0.2)V_(Ni0.1)Ru_(0.3)Mn_(0.4)]O_(2)(V-NRM)compound.Various analytical techniques including transmission electron microscopy,X-ray absorption near edge spectroscopy,operando X-ray diffraction,and operando differential electrochemical mass spectrometry are employed to assess changes in the average oxidation states and structural distortions.The results demonstrate that V-NRM exhibits higher capacity than NRM and maintains a moderate capacity retention of 81%after 100 cycles.Furthermore,the formation of additional lone-pair electrons in the O 2p orbital enables V-NRM to utilize more capacity from the oxygen redox validated by density functional calculation,leading to a widened dominance of the OP4 phase without releasing O_(2) gas.These findings offer valuable insights for the design of advanced high-capacity cathode materials with improved performance and sustainability in sodium-ion batteries. 展开更多
关键词 Layered oxide Oxygen evolution Sodium battery VACANCY CATHODE
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Precisely Control Relationship between Sulfur Vacancy and H Absorption for Boosting Hydrogen Evolution Reaction 被引量:1
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作者 Jing Jin Xinyao Wang +4 位作者 Yang Hu Zhuang Zhang Hongbo Liu Jie Yin Pinxian Xi 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第4期14-24,共11页
Ef fective and robust catalyst is the core of water splitting to produce hydrogen.Here, we report an anionic etching method to tailor the sulfur vacancy(VS) of NiS_(2) to further enhance the electrocatalytic performan... Ef fective and robust catalyst is the core of water splitting to produce hydrogen.Here, we report an anionic etching method to tailor the sulfur vacancy(VS) of NiS_(2) to further enhance the electrocatalytic performance for hydrogen evolution reaction(HER). With the VS concentration change from 2.4% to 8.5%, the H* adsorption strength on S sites changed and NiS_(2)-VS 5.9% shows the most optimized H* adsorption for HER with an ultralow onset potential(68 m V) and has long-term stability for 100 h in 1 M KOH media. In situ attenuated-total-reflection Fourier transform infrared spectroscopy(ATR-FTIRS) measurements are usually used to monitor the adsorption of intermediates. The S-H* peak of the Ni S_(2)-VS 5.9% appears at a very low voltage, which is favorable for the HER in alkaline media. Density functional theory calculations also demonstrate the Ni S_(2)-VS 5.9% has the optimal |ΔG^(H*)| of 0.17 e V. This work offers a simple and promising pathway to enhance catalytic activity via precise vacancies strategy. 展开更多
关键词 Hydrogen evolution reaction S vacancies NANOSHEET H Adsorption
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Unsaturated bi-heterometal clusters in metal-vacancy sites of 2D MoS2 for efficient hydrogen evolution 被引量:1
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作者 Gonglei Shao Jie Xu +4 位作者 Shasha Gao Zhang Zhang Song Liu Xu Zhang Zhen Zhou 《Carbon Energy》 SCIE EI CAS CSCD 2024年第3期264-275,共12页
The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clu... The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum disulfide.The unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active sites.Among them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical calculation.Whereupon,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials. 展开更多
关键词 CLUSTERS hydrogen evolution reaction metal vacancy MOS2 unsaturated heterometal
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Defect engineering in transition-metal(Fe,Co,andNi)-based electrocatalysts for water splitting 被引量:1
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作者 Kaili Wu Chaojie Lyu +5 位作者 Jiarun Cheng Weifan Ding Jiwen Wu Qian Wang Woon-Ming Lau Jinlong Zheng 《Carbon Energy》 SCIE EI CAS CSCD 2024年第6期165-199,共35页
Electrocatalytic water splitting seems to be an efficient strategy to deal with increasingly serious environmental problems and energy crises but still suffers from the lack of stable and efficient electrocatalysts.De... Electrocatalytic water splitting seems to be an efficient strategy to deal with increasingly serious environmental problems and energy crises but still suffers from the lack of stable and efficient electrocatalysts.Designing practical electrocatalysts by introducing defect engineering,such as hybrid structure,surface vacancies,functional modification,and structural distortions,is proven to be a dependable solution for fabricating electrocatalysts with high catalytic activities,robust stability,and good practicability.This review is an overview of some relevant reports about the effects of defect engineering on the electrocatalytic water splitting performance of electrocatalysts.In detail,the types of defects,the preparation and characterization methods,and catalytic performances of electrocatalysts are presented,emphasizing the effects of the introduced defects on the electronic structures of electrocatalysts and the optimization of the intermediates'adsorption energy throughout the review.Finally,the existing challenges and personal perspectives of possible strategies for enhancing the catalytic performances of electrocatalysts are proposed.An in-depth understanding of the effects of defect engineering on the catalytic performance of electrocatalysts will light the way to design high-efficiency electrocatalysts for water splitting and other possible applications. 展开更多
关键词 defect engineering electrocatalytic water splitting element doping interfacial engineering VACANCY
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Engineering of oxygen vacancy and bismuth cluster assisted ultrathin Bi_(12)O_(17)Cl_(2)nanosheets with efficient and selective photoreduction of CO_(2)to CO 被引量:2
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作者 Meili Guan Ni Lu +7 位作者 Xuan Zhang Qiuwan Wang Jian Bao Guiye Chen Hao Yu Huaming Li Jiexiang Xia Xuezhong Gong 《Carbon Energy》 SCIE EI CAS CSCD 2024年第4期1-11,共11页
The photocatalytic conversion of CO_(2)into solar‐powered fuels is viewed as a forward‐looking strategy to address energy scarcity and global warming.This work demonstrated the selective photoreduction of CO_(2)to C... The photocatalytic conversion of CO_(2)into solar‐powered fuels is viewed as a forward‐looking strategy to address energy scarcity and global warming.This work demonstrated the selective photoreduction of CO_(2)to CO using ultrathin Bi_(12)O_(17)Cl_(2)nanosheets decorated with hydrothermally synthesized bismuth clusters and oxygen vacancies(OVs).The characterizations revealed that the coexistences of OVs and Bi clusters generated in situ contributed to the high efficiency of CO_(2)–CO conversion(64.3μmol g^(−1)h^(−1))and perfect selectivity.The OVs on the facet(001)of the ultrathin Bi_(12)O_(17)Cl_(2)nanosheets serve as sites for CO_(2)adsorption and activation sites,capturing photoexcited electrons and prolonging light absorption due to defect states.In addition,the Bi‐cluster generated in situ offers the ability to trap holes and the surface plasmonic resonance effect.This study offers great potential for the construction of semiconductor hybrids as multiphotocatalysts,capable of being used for the elimination and conversion of CO_(2)in terms of energy and environment. 展开更多
关键词 Bi cluster Bi_(12)O_(17)Cl_(2)nanosheet oxygen vacancy photocatalytic CO_(2)reduction
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Universal architecture and defect engineering dual strategy for hierarchical antimony phosphate composite toward fast and durable sodium storage 被引量:1
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作者 Jiawei Wu Gaoyu Wang +7 位作者 Wei Zhang Lixiang Wang Jian Peng Qinghua Li Zhixin Liang Wenbo Fan Jiazhao Wang Shaoming Huang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第3期110-119,I0004,共11页
Antimony(Sb)-ba sed anode materials are feasible candidates for sodium-ion batteries(SIBs) due to their high theoretical specific capacity and excellent electrical conductivity.However,they still suffer from volume di... Antimony(Sb)-ba sed anode materials are feasible candidates for sodium-ion batteries(SIBs) due to their high theoretical specific capacity and excellent electrical conductivity.However,they still suffer from volume distortion,structural collapse,and ionic conduction interruption upon cycling.Herein,a hierarchical array-like nanofiber structure was designed to address these limitations by combining architecture engineering and anion tuning strategy,in which SbPO_(4-x) with oxygen vacancy nanosheet arrays are anchored on the surface of interwoven carbon nanofibers(SbPO_(4-x)@CNFs).In particular,bulky PO_(4)^(3-) anions mitigate the large volume distortion and generate Na_(3)PO_(4) with high ionic conductivity,collectively improving cyclic stability and ionic transport efficiency.The abundant oxygen vacancies substantially boost the intrinsic electronic conductivity of SbPO_4,further accelerating the reaction dynamics.In addition,hierarchical fibrous structures provide abundant active sites,construct efficient conducting networks,and enhance the electron/ion transport capacity.Benefiting from the advanced structural design,the SbPO_(4-x)@CNFs electrodes exhibit outstanding cycling stability(1000 cycles at 1.0 A g^(-1) with capacity decay of 0.05% per cycle) and rapid sodium storage performance(293.8 mA h g^(-1) at 5.0 A g^(-1)).Importantly,systematic in-/ex-situ techniques have revealed the "multi-step conversion-alloying" reaction process and the "battery-capacitor dual-mode" sodium-storage mechanism.This work provides valuable insights into the design of anode materials for advanced SIBs with elevated stability and superior rate performance. 展开更多
关键词 SbPO_(4) anodes Hierarchical nanostructures Oxygen vacancy Stress dispersion Sodium-ion batteries
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Bifunctional TiO_(2-x)nanofibers enhanced gel polymer electrolyte for high performance lithium metal batteries 被引量:1
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作者 Yixin Wu Zhen Chen +6 位作者 Yang Wang Yu Li Chunxing Zhang Yihui Zhu Ziyu Yue Xin Liu Minghua Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第2期437-448,I0011,共13页
Exploration of advanced gel polymer electrolytes(GPEs)represents a viable strategy for mitigating dendritic lithium(Li)growth,which is crucial in ensuring the safe operation of high energy density Li metal batteries(L... Exploration of advanced gel polymer electrolytes(GPEs)represents a viable strategy for mitigating dendritic lithium(Li)growth,which is crucial in ensuring the safe operation of high energy density Li metal batteries(LMBs).Despite this,the application of GPEs is still hindered by inadequate ionic conductivity,low Li^(+)transference number,and subpar physicochemical properties.Herein,Ti O_(2-x)nanofibers(NF)with oxygen vacancy defects were synthesized by a one-step process as inorganic fillers to enhance the thermal/mechanical/ionic-transportation performances of composite GPEs.Various characterizations and theoretical calculations reveal that the oxygen vacancies on the surface of Ti O_(2-x)NF accelerate the dissociation of Li PF_6,promote the rapid transfer of free Li^(+),and influence the formation of Li F-enriched solid electrolyte interphase.Consequently,the composite GPEs demonstrate enhanced ionic conductivity(1.90m S cm^(-1)at room temperature),higher lithium-ion transference number(0.70),wider electrochemical stability window(5.50 V),superior mechanical strength,excellent thermal stability(210℃),and improved compatibility with lithium,resulting in superior cycling stability and rate performance in both Li||Li,Li||Li Fe PO_(4),and Li||Li Ni_(0.8)Co_(0.1)Mn_(0.1)O_(2)cells.Overall,the synergistic influence of nanofiber morphology and enriched oxygen vacancy structure of fillers on electrochemical properties of composite GPEs is comprehensively investigated,thus,it is anticipated to shed new light on designing high-performance GPEs LMBs. 展开更多
关键词 Nanofibers fillers Oxygen vacancies Gel polymer electrolytes Lithium metal batteries
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Investigating the impact of dynamic structural changes of Au/rutile catalysts on the catalytic activity of CO oxidation 被引量:1
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作者 Xiaochun Hu Qianwenhao Fan +9 位作者 Mingwu Tan Yuqing Luo Xianyue Wu Manoel Y.Manuputty Jie Ding Tej S.Choksi Markus Kraft Rong Xu Zhiqiang Sun Wen Liu 《Carbon Energy》 SCIE EI CAS CSCD 2024年第4期222-232,共11页
The surface properties of oxidic supports and their interaction with the supported metals play critical roles in governing the catalytic activities of oxide‐supported metal catalysts.When metals are supported on redu... The surface properties of oxidic supports and their interaction with the supported metals play critical roles in governing the catalytic activities of oxide‐supported metal catalysts.When metals are supported on reducible oxides,dynamic surface reconstruction phenomena,including strong metal–support interaction(SMSI)and oxygen vacancy formation,complicate the determination of the structural–functional relationship at the active sites.Here,we performed a systematic investigation of the dynamic behavior of Au nanocatalysts supported on flame‐synthesized TiO_(2),which takes predominantly a rutile phase,using CO oxidation above room temperature as a probe reaction.Our analysis conclusively elucidated a negative correlation between the catalytic activity of Au/TiO_(2) and the oxygen vacancy at the Au/TiO_(2) interface.Although the reversible formation and retracting of SMSI overlayers have been ubiquitously observed on Au/TiO_(2) samples,the catalytic consequence of SMSI remains inconclusive.Density functional theory suggests that the electron transfer from TiO_(2) to Au is correlated to the presence of the interfacial oxygen vacancies,retarding the catalytic activation of CO oxidation. 展开更多
关键词 CO oxidation electronic metal-support interactions flame‐synthesis metal-support interactions oxygen vacancy strong metal-support interaction
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Excess Activity Tuned by Distorted Tetrahedron in CoMoO_(4) for Oxygen Evolution 被引量:1
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作者 Hengbo Xiao Kai Chi +10 位作者 Hongxia Yin Xiangji Zhou Pengxiang Lei Peizhi Liu Jiakun Fang Xiuhong Li Songliu Yuan Zhen Zhang Yaqiong Su Junjie Guo Lihua Qian 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第1期247-252,共6页
Oxygen vacancies enable modulating surface reconstruction of transition metal oxides containing metal-oxygen polyhedrons into metallic oxyhydroxide for oxygen evolution reaction(OER),while revealing reconstructing mec... Oxygen vacancies enable modulating surface reconstruction of transition metal oxides containing metal-oxygen polyhedrons into metallic oxyhydroxide for oxygen evolution reaction(OER),while revealing reconstructing mechanism is stuck by the requirement to precisely control exact sites of these vacancies.Herein,oxygen vacancies are localized only within MoO_(4)tetrahedrons rather than CoO_(6)octahedrons in CoMoO_(4)catalyst,guaranteeing coherent reconstruction of CoO_(6)octahedrons into pure CoOOH with tunable activities for OER.Meanwhile,distorted tetrahedron accelerates the dissolution of Mo atoms into alkaline electrolyte,triggering spontaneous transition of partial CoMoO_(4)into Co(OH)_(2).CoO_(6)octahedrons in both CoMoO_(4)and Co(OH)_(2)can transform pure CoOOH completely at lower potential,resulting in excess intrinsic activity whose summit is identified by overpotential at 10 mA cm^(-2)with 22.9%reduction and Tafel slope with 65.3%reduction.Well-defined manipulation over the distorted polyhedrons offers one versatile knob to precisely modulate electronic structure of oxide catalysts with outstanding OER performance. 展开更多
关键词 metal-oxygen polyhedron oxygen evolution reaction oxygen vacancy Raman spectroscopy
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Effects of vacancy and external electric field on the electronic properties of the MoSi_(2)N_(4)/graphene heterostructure 被引量:1
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作者 梁前 罗祥燕 +3 位作者 钱国林 王远帆 梁永超 谢泉 《Chinese Physics B》 SCIE EI CAS CSCD 2024年第3期542-550,共9页
Recently,the newly synthesized septuple-atomic layer two-dimensional(2D)material MoSi_(2)N_(4)(MSN)has attracted attention worldwide.Our work delves into the effect of vacancies and external electric fields on the ele... Recently,the newly synthesized septuple-atomic layer two-dimensional(2D)material MoSi_(2)N_(4)(MSN)has attracted attention worldwide.Our work delves into the effect of vacancies and external electric fields on the electronic properties of the MSN/graphene(Gr)heterostructure using first-principles calculation.We find that four types of defective structures,N-in,N-out,Si and Mo vacancy defects of monolayer MSN and MSN/Gr heterostructure are stable in air.Moreover,vacancy defects can effectively modulate the charge transfer at the interface of the MSN/Gr heterostructure as well as the work function of the pristine monolayer MSN and MSN/Gr heterostructure.Finally,the application of an external electric field enables the dynamic switching between n-type and p-type Schottky contacts.Our work may offer the possibility of exceeding the capabilities of conventional Schottky diodes based on MSN/Gr heterostructures. 展开更多
关键词 MoSi_(2)N_(4) vacancy defects external electric field Schottky contacts
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Borohydride Ammoniate Solid Electrolyte Design for All-Solid-State Mg Batteries 被引量:1
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作者 Yuepeng Pang Zhengfang Nie +5 位作者 Fen Xu Lixian Sun Junhe Yang Dalin Sun Fang Fang Shiyou Zheng 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第1期100-106,共7页
Searching for novel solid electrolytes is of great importance and challenge for all-solid-state Mg batteries.In this work,we develop an amorphous Mg borohydride ammoniate,Mg(BH_(4))_(2)·2NH_(3),as a solid Mg elec... Searching for novel solid electrolytes is of great importance and challenge for all-solid-state Mg batteries.In this work,we develop an amorphous Mg borohydride ammoniate,Mg(BH_(4))_(2)·2NH_(3),as a solid Mg electrolyte that prepared by a NH_(3)redistribution between 3D framework-γ-Mg(BH_(4))_(2)and Mg(BH_(4))_(2)·6NH_(3).Amorphous Mg(BH_(4))_(2)·2NH_(3)exhibits a high Mg-ion conductivity of 5×10^(-4)S cm^(-1)at 75℃,which is attributed to the fast migration of abundant Mg vacancies according to the theoretical calculations.Moreover,amorphous Mg(BH_(4))_(2)·2NH_(3)shows an apparent electrochemical stability window of 0-1.4 V with the help of in-situ formed interphases,which can prevent further side reactions without hindering the Mg-ion transfer.Based on the above superiorities,amorphous Mg(BH_(4))_(2)·2NH_(3)enables the stable cycling of all-solid-state Mg cells,as the critical current density reaches 3.2 mA cm^(-2)for Mg symmetrical cells and the reversible specific capacity reaches 141 mAh g^(-1)with a coulombic efficiency of 91.7%(first cycle)for Mg||TiS_(2)cells. 展开更多
关键词 all-solid-state Mg batteries amorphization Mg borohydride ammoniate Mg vacancy migration solid electrolyte
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Bimetallic In_(2)O_(3)/Bi_(2)O_(3) Catalysts Enable Highly Selective CO_(2) Electroreduction to Formate within Ultra-Broad Potential Windows 被引量:1
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作者 Zhongxue Yang Hongzhi Wang +7 位作者 Xinze Bi Xiaojie Tan Yuezhu Zhao Wenhang Wang Yecheng Zou Huai ping Wang Hui Ning Mingbo Wu 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第1期257-264,共8页
CO_(2)electrochemical reduction reaction(CO_(2)RR)to formate is a hopeful pathway for reducing CO_(2)and producing high-value chemicals,which needs highly selective catalysts with ultra-broad potential windows to meet... CO_(2)electrochemical reduction reaction(CO_(2)RR)to formate is a hopeful pathway for reducing CO_(2)and producing high-value chemicals,which needs highly selective catalysts with ultra-broad potential windows to meet the industrial demands.Herein,the nanorod-like bimetallic ln_(2)O_(3)/Bi_(2)O_(3)catalysts were successfully synthesized by pyrolysis of bimetallic InBi-MOF precursors.The abundant oxygen vacancies generated from the lattice mismatch of Bi_(2)O_(3)and ln_(2)O_(3)reduced the activation energy of CO_(2)to*CO_(2)·^(-)and improved the selectivity of*CO_(2)·^(-)to formate simultaneously.Meanwhile,the carbon skeleton derived from the pyrolysis of organic framework of InBi-MOF provided a conductive network to accelerate the electrons transmission.The catalyst exhibited an ultra-broad applied potential window of 1200 mV(from-0.4 to-1.6 V vs RHE),relativistic high Faradaic efficiency of formate(99.92%)and satisfactory stability after 30 h.The in situ FT-IR experiment and DFT calculation verified that the abundant oxygen vacancies on the surface of catalysts can easily absorb CO_(2)molecules,and oxygen vacancy path is dominant pathway.This work provides a convenient method to construct high-performance bimetallic catalysts for the industrial application of CO_(2)RR. 展开更多
关键词 bimetallic catalyst CO_(2)electrochemical reduction reaction FORMATE oxygen vacancy wide potential window
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Chemically bonded Mn_(0.5)Cd_(0.5)S/BiOBr S-scheme photocatalyst with rich oxygen vacancies for improved photocatalytic decontamination performance 被引量:2
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作者 Shijie Li Changjun You +3 位作者 Ke Rong Chunqiang Zhuang Xiaobo Chen Bin Zhang 《Advanced Powder Materials》 2024年第3期12-22,共11页
Devising exceptional S-scheme heterojunction photocatalysts utilized in annihilating pharmaceuticals and chromium contamination is significant for addressing the problem of global water pollution.In this work,a chemic... Devising exceptional S-scheme heterojunction photocatalysts utilized in annihilating pharmaceuticals and chromium contamination is significant for addressing the problem of global water pollution.In this work,a chemically bonded Mn0.5Cd_(0.5)S/BiOBr S-scheme heterostructure with oxygen vacancies is ingeniously developed through a facile in-situ solvothermal synthesis.The designed Mn0.5Cd_(0.5)S/BiOBr heterojunction exhibits eminently reinforced photo-activity for destruction of tetracycline hydrochloride and Cr(VI)as compared with its individual components.This substantial photo-redox performance amelioration is benefitted from the creation of an intense internal electric field(IEF)via supplying powerful driving force and migration highway by interfacial chemical bond to foster the S-scheme electron/hole disintegration.More intriguingly,the IEF at the hetero-interface drives the fast consumption of the photo-induced holes in Mn0.5Cd_(0.5)S by the photoelectrons from BiOBr,profoundly boosting the enrichment of active photo-carriers and sparing the photo-corrosion of Mn0.5Cd_(0.5)S.Furthermore,Mn0.5Cd_(0.5)S/BiOBr with exceptional anti-interference property can work efficiently in real water matrices.Multiple uses of the recycled Mn0⋅5Cd0⋅5S/BiOBr evidence its prominent robustness and stability.This achievement indicates the vast potential of chemically bonded S-scheme photosystems with structural defects in the design of photo-responsive materials for effective wastewater treatment. 展开更多
关键词 Mn_(0.5)Cd_(0⋅5)S/BiOBr Chemically bonded S-Scheme Internal electric field Oxygen vacancies Antibiotic removal Photocatalysis
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Solution-flame hybrid synthesis of defect-enriched mesoporous CuO_(x) nanowires for enhanced electrochemical nitrate-to-ammonia production
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作者 Li Qu Sungkyu Kim +7 位作者 Runfa Tan Arumugam Sivanantham Seokgi Kim Yoo Jae Jeong Min Cheol Kim Seong Sik Shin Uk Sim In Sun Cho 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第12期475-483,共9页
Electrochemical nitrate reduction(ENR)is an economical and eco-friendly method for converting industrial wastewater into valuable ammonia under atmospheric conditions.The main challenge lies in designing and developin... Electrochemical nitrate reduction(ENR)is an economical and eco-friendly method for converting industrial wastewater into valuable ammonia under atmospheric conditions.The main challenge lies in designing and developing highly durable ENR electrocatalysts.This study introduces defect-rich mesoporous CuO_(x) nanowires electrocatalyst synthesized using a novel solution-flame(sol-flame)hybrid method to control mesoporosity and introduce surface defects,thereby enhancing the electrochemical nitrate-toammonia production performance.We found surface defects(oxygen vacancies and Cu^(+))and unique mesoporous nanowire structure composed of tightly interconnected nanoparticles.The sol-flamesynthesized CuO_(x) nanowires(sf-CuO NWs)achieved superior ammonia yield rate(0.51 mmol h^(-1)cm^(-2)),faradaic efficiency(97.3%),and selectivity(86.2%)in 1 M KOH electrolyte(2000 ppm nitrate).This performance surpasses that of non-porous and less-defective CuO NWs and is attributed to the increased surface area and rapid electron transport facilitated by the distinctive morphology and generated defects.Theoretical calculation further suggests oxygen vacancies enhance NO_(3)^(-)adsorption on the sf-CuO NWs’surface and mitigate the competing hydrogen evolution reaction.This study outlines a strategic design and simple synthesis approach for nanowire electrocatalysts that boost the efficiency of electrochemical nitrate-to-ammonia conversion. 展开更多
关键词 CuO nanowires Solution-flame MESOPOROUS Oxygen vacancy Electrochemical nitrate reduction Wastewater
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Insights into Reduction of CO_(2)to CO Catalyzed by Pyramidal-4Ni Clusters Supported on Doped CeO_(2)
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作者 Ruimin Qin Shenyu Shen +4 位作者 Boyang Li Tingyi Zhu Tiantian Wu Shujiang Ding Yaqiong Su 《Chinese Journal of Chemical Physics》 SCIE EI CAS CSCD 2024年第5期591-598,I0028-I0037,I0099,共19页
Converting CO_(2)into valuable chemicals has become a widely used research method for CO_(2)conversion.In this work,the catalytic performance of pyramidal-4Ni catalysts supported on rare earth metal-doped CeO_(2)towar... Converting CO_(2)into valuable chemicals has become a widely used research method for CO_(2)conversion.In this work,the catalytic performance of pyramidal-4Ni catalysts supported on rare earth metal-doped CeO_(2)towardCO_(2)reductionreaction(CO_(2)RR)was investigated by using density-functional theorycalculations.For rare earth metal-doped CeO_(2),2Ce is substituted by 2 trivalent cations and at the same time one oxygen vacancy is created to make charge compensation.We investigated the oxygen vacancy nearest(Vo,N)and next-nearest(Vo,NN)to 4Ni,and found releasing CO and CO_(2)dissociation are the rate-determining steps,respectively,via the path of Vo,N and Vo,NN.Among the studied dopants(Ga,Sb,Lu,Gd,Pr,La,Bi),Gd is identified as the best dopant for catalyzing the reduction of CO_(2)at 823 K,with the turn-over frequency(TOF)of 104 times as large as that over 4Ni supported on pure CeO_(2).This exploration provides theoretical support and guidance for the research and application of rare earth metaldoped CeO_(2)-loaded Ni catalysts in the field of CO_(2)reduction. 展开更多
关键词 Carbon dioxide reduction CeO_(2)(111) Oxygen VACANCY Density functional theory
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Oxygen vacancy-boosted thermocatalytic CO_(2) hydrogenation:Engineering strategies,promoting effects and mediating mechanisms
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作者 Guiming Xie Xiaorui Wang +3 位作者 Xianfeng Li Yunming Fang Runduo Zhang Zhou-jun Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第12期393-408,共16页
Thermocatalytic CO_(2) hydrogenation with"green"H_(2) is one of the most promising carbon-negative technologies,wherein oxygen vacancy engineering serves as a novel strategy to boost the catalytic performanc... Thermocatalytic CO_(2) hydrogenation with"green"H_(2) is one of the most promising carbon-negative technologies,wherein oxygen vacancy engineering serves as a novel strategy to boost the catalytic performance of oxide-containing catalysts.To provide theoretical guidance and promote technical progress in this important field,the status and prospect of oxygen vacancy-boosted thermocatalytic CO_(2) hydrogenation have been thoroughly reviewed herein.Specifically,fundamentals including origin,construction,characterization,and function of oxygen vacancies will be systematically summarized and oxygen vacancy-boosted hydrogenation reactions including methanation,reverse water-gas shift(RWGS),methanol synthesis,and other hydrogenation processes will be comprehensively introduced.In addition,challenges and opportunities from the perspective of engineering strategies,promoting effects,and mediating mechanisms of oxygen vacancies will be succinctly proposed.Overall,this review is expected to gain more insights into the role of oxygen vacancies and shed new light on the design of efficient oxide-containing catalysts. 展开更多
关键词 Oxygen vacancies Carbon dioxide Hydrogen Thermocatalysis Oxide-containing catalysts
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