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Unsaturated bi-heterometal clusters in metal-vacancy sites of 2D MoS2 for efficient hydrogen evolution

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Carbon Energy 2024年第3期6卷 264-275页

作者： Gonglei Shao Jie Xu Shasha Gao Zhang Zhang Song Liu Xu Zhang Zhen Zhou Interdisciplinary research center for Sustainable Energy Science and engineering(IRC4SE2) School of Chemical EngineeringZhengzhou UniversityZhengzhouHenanChina college of chemistry and Materials engineering Wenzhou UniversityWenzhouZhejiangChina Key Laboratory of advanced Energy Materials chemistry(ministry of education) College of ChemistryNankai UniversityTianjinChina State Key Laboratory of Chemo/Biosensing and Chemometrics Institute of Chemical Biology and Nanomedicine(ICBN)College of Chemistry and Chemical EngineeringHunan UniversityChangshaHunanChina Institute of New Energy Material chemistry School of Materials Science and EngineeringNankai UniversityTianjinChina

The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation ***,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 *** 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 *** 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 ***,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.

关键词： clusters hydrogen evolution reaction metal vacancy MoS2 unsaturated heterometal

Molecular surface functionalization of In_(2)O_(3) to tune interfacial microenvironment for enhanced catalytic performance of CO_(2) electroreduction

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Nano research 2024年第3期17卷 1242-1250页

作者： Suwen WangQiang GaoCui Xu Shuai Jiang Mengyang Zhang Xianjun Yin Hui-Qing Peng Bin Liu Yu-Fei Song State Key Laboratory of chemical Resource engineering Beijing Advanced Innovation Center for Soft Matter Science and EngineeringCollege of ChemistryBeijing University of Chemical TechnologyBeijing 100029China

Indium-based materials(e.g.,In_(2)O_(3))are a class of promising non-noble metal-based catalysts for electroreduction of carbon dioxide(CO_(2)).However,competitive hydrogen reduction reaction(HER)on indium-based catalysts hampers CO_(2) reduction reaction(CO_(2)RR)*** herein tune the interfacial microenvironment of In_(2)O_(3) through chemical graft of alkyl phosphoric acid molecules using a facile solution-processed strategy for the first time,which is distinguished from other researches that tailor intrinsic activity of In_(2)O_(3) *** surface functionalization of alkyl phosphoric acids over In_(2)O_(3) is demonstrated to remarkably boost CO_(2) *** example,octadecylphosphonic acid modified In_(2)O_(3) exhibits Faraday efficiency for H_(2) H_(2) H_(2)(FE)of as low as 6.6%and FEHCOOH of 86.5%at-0.67 V ***,which are far superior to parent In_(2)O_(3) counterparts(FE of 24.0%and FEHCOOH of 63.1%).Moreover,the enhancing effect of alkyl phosphoric acid functionalization is found to be closely related to the length of alkyl *** virtue of comprehensive experimental characterizations and molecular dynamics simulations,it is revealed that the modification of alkyl phosphoric acids significantly alters the interface microenvironment of the electrocatalyst,which changes the electrocatalyst surface from hydrophilic and aerophobic to hydrophobic and *** this case,the water molecules are pushed away and more CO_(2) molecules are trapped,increasing local CO_(2) concentration at In_(2)O_(3) active sites,thus leading to the significantly enhanced CO_(2)RR and suppressed *** work highlights the importance of regulating the interfacial microenvironment of inorganic catalysts by molecular surface functionalization as a means for promoting the electrochemical performance in electrosynthesis and beyond.

关键词： carbon dioxide(CO_(2))electroreduction interfacial microenvironment molecular surface functionalization In_(2)O_(3)catalyst water and CO_(2)diffusion

Bifunctional core–shell co-catalyst for boosting photocatalytic CO_(2) reduction to CH_(4)

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Nano research 2024年第3期17卷 1259-1266页

作者： Fangxu Dai Mingming Zhang Jishu Han Zhenjiang Li Shouhua Feng Jun Xing Lei Wang Key Laboratory of Eco-chemical engineering Ministry of EducationCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China college of Materials Science and engineering Qingdao University of Science and TechnologyQingdao 266042China college of Environment and Safety engineering Qingdao University of Science and TechnologyShandong Engineering Research Center for Marine Environment Corrosion and Safety ProtectionQingdao 266042China

Solar-light-driven CO_(2) reduction CO to CH_(4) and C2H6 is a complex process involving multiple elementary reactions and energy ***,achieving high CH_(4) activity and selectivity remains a significant ***,we integrate bifunctional Cu2O and Cu-MOF(MOF=metal-organic framework)core–shell co-catalysts(Cu2O@Cu-MOF)with semiconductor TiO_(2).Experiments and theoretical calculations demonstrate that Cu2O(Cu+facilitates charge separation)and Cu-MOF(Cu2+improves the CO_(2) adsorption and activation)in the core–shell structure have a synergistic effect on photocatalytic CO_(2) reduction,reducing the formation barrier of the key intermediate*COOH and**** photocatalyst exhibits high CH_(4) yield(366.0μmol·g^(-1)·h^(-1)),efficient electron transfer(3283μmol·g^(-1)·h^(-1))and hydrocarbon selectivity(95.5%),which represents the highest activity of Cu-MOF-based catalysts in photocatalytic CO_(2) reduction *** work provides a strategy for designing efficient photocatalysts from the perspective of precise regulation of components.

关键词： bifunctional co-catalyst core–shell photocatalytic CO_(2)reduction

Synergism of solar-driven interfacial evaporation and photo-Fenton Cr(Ⅵ) reduction by sustainable Bi-MOF-based evaporator from waste polyester

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Journal of Energy chemistry 2024年第7期94卷 527-540页

作者： Zifen Fan Jie Liu Huajian Liu Lijie Liu Yan She Xueying Wen Huiyue Wang Guixin Hu Ran Niu Jiang Gong Key Laboratory of Material chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureHubei Engineering Research Center for Biomaterials and Medical Protective MaterialsSemiconductor Chemistry CenterSchool of Chemistry and Chemical EngineeringHuazhong University of Science andTechnologyWuhan430074HubeiChina

The integration of interfacial solar steam generation and photocatalytic degradation technology has pro-vided a promising platform to simultaneously produce freshwater and degrade ***,con-structing low-cost,multi-functional evaporators for treating Cr(Ⅵ)-polluted water remains challenging,and the synergistic mechanism on Cr(Ⅵ)reduction is ***,we propose the combined strategy of ball milling and solution mixing for the sustainable production of Bi-MOF microrod from waste poly(ethylene terephthalate),and construct Bi-MOF-based solar evaporators for simultaneous photo-Fenton Cr(Ⅵ)reduction and freshwater ***,the evaporator comprised of Bi-MOF microrod and graphene nanosheet possesses high light absorption,efficient photothermal conversion,and good hydro-philic *** to the advantages,the hybrid evaporator exhibits the evaporation rate of 2.16 kg m^(-2) h^(-1) and evaporation efficiency of 87.5%under 1 kW m^(-2) of *** integrating with photo-Fenton reaction,the Cr(Ⅵ)reduction efficiency is 91.3%,along with the reaction kinetics of 0.0548 min^(-1),surpassing many advanced *** the outdoor freshwater production and Cr(Ⅵ)reduction,the daily accumulative water yield is 5.17 kg m^(-2) h^(-1),and the Cr(Ⅵ)reduction efficiency is 99.9%.Furthermore,we prove that the localization effect derived from the interfacial solar-driven evap-oration enhances H_(2)O_(2) activation for the photo-Fenton reduction of Cr(Ⅵ).Based on the result of density functional theory,Bi-MOF microrod provides rich active centers for H_(2)O_(2) activation to produce active sites such as e-or-O_(2).This study not only proposes a new strategy to construct multi-functional solar evaporators for freshwater production and catalytic reduction of pollutants,but also advances the chem-ical upcycling of waste polyesters.

关键词： Interfacial solar steam generation Cr(VI)reduction Photo-Fenton reaction Metal-organic framework Waste plastic upcycling

A healable, mechanically robust and ultrastretchable ionic conductive elastomer for durably wearable sensor

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Nano research 2024年第4期17卷 3369-3378页

作者： Guoxian Zhang Chunmei Li JiaoJun Tan Mingqi Wang Yafeng Ren Feijie Ge Qiuyu Zhang 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 college of Bioresources chemical and Materials engineering National Demonstration Center for Experimental Light Chemistry Engineering EducationShaanxi University of Science&TechnologyXi’an 710021China

The ionic conductive elastomers show great promise in multifunctional wearable electronics,but they currently suffer from liquid leakage/evaporation or mechanical *** ionic conductive elastomers integrating non-volatility,mechanical robustness,superior ionic conductivity,and ultra-stretchability remains urgent and ***,we developed a healable,robust,and conductive elastomer via impregnating free ionic liquids(ILs)into the ILs-multigrafted poly(urethane-urea)(PUU)elastomer networks.A crucial strategy in the molecular design is that imidazolium cations are largely introduced by double-modification of PUU and centipede-like structures are obtained,which can lock the impregnated ILs through strong ionic *** this system,the PUU matrix contributes outstanding mechanical properties,while the hydrogen bonds and ionic interactions endow the elastomer with self-healing ability,conductivity,as well as non-volatility and *** fabricated ionic conductive elastomers show good conductivity(3.8×10^(-6) S·cm^(-1)),high mechanical properties,including tensile stress(4.64 MPa),elongation(1470%),and excellent healing ability(repairing efficiency of 90%after healing at room temperature for 12 h).Significantly,the conductive elastomers have excellent antifatigue properties,and demonstrate a highly reproducible response after 1000 uninterrupted extension-release *** work provides a promising strategy to prepare ionic conductive elastomers with excellent mechanical properties and stable sensing capacity,and further promote the development of mechanically adaptable intelligent sensors.

关键词： ionic conductive elastomers poly(urethane-urea)(PUU) ionic interactions centipede-like self-healing

Heterostructure:application of absorption-catalytic center in lithium-sulfur batteries

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Rare Metals 2024年第4期43卷 1461-1487页

作者： Fei Wang Chun-Man Yang Yong-Qi Wang Dan You Wen-Hao Yang Rong-Wei Huang Ji-Yue Hou Qian Wang Ying-Jie Zhang Ying Wang Yue-Jing Zeng Yi-Yong Zhang Xue Li National Local Joint engineering research center for Lithium-Ion Batteries and Materials Preparation Technology Key Laboratory of Advanced Batteries Materials of Yunnan ProvinceFaculty of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunming650093China college of Electrical Information engineering Panzhihua UniversityPanzhihua617000China State Key Laboratory of Physical chemistry of Solid Surfaces Collaborative Innovation Centre of Chemistry for Energy MaterialsState-Province Joint Engineering Laboratory of Power Source Technology for New Energy VehicleEngineering Research Center of Electrochemical TechnologyMinistry of EducationCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China

Due to the high theoretical specific capacity(1675 mAh·g^(-1)),low cost,and high safety of the sulfur cathodes,they are expected to be one of the most promising rivals for a new generation of energy storage ***,the shuttle effect,low conductivity of sulfur and its discharge products,volume expansion,and other factors hinder the commercialization of lithium-sulfur batteries(LSBs).The development of sulfur-fixing materials and the design of multifunctional materials to enhance the electrochemical performance of LSBs have been the main research priorities in recent *** of the advantages of high conductivity,built-in electric field,and good synergism,more and more researchers have employed heterostructure into sulfur-fixing materials to enhance the catalytic and absorption ability for *** this review,the principle of heterostructure and the mechanism of enhancing the performance of lithium-sulfur batteries are *** applications of heterostructure in cathode and interlayer of LSBs in the latest years are ***,the cutting-edge troubles and possibilities of heterostructures in LSBs are briefly presented.

关键词： Lithium-sulfur batteries(LSBs) Heterostructure Built-in electric field catalytic Absorption

An efficient and mild recycling of waste melamine formaldehyde foams by alkaline hydrolysis

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Green Energy & Environment 2024年第5期9卷 919-926页

作者： Shaodi Wu Ning Zhang Chizhou Wang Xianglin Hou Jie Zhao Shiyu Jia Jiancheng Zhao Xiaojing Cui Haibo Jin Tiansheng Deng Shanxi engineering research center of Biorefinery Institute of Coal ChemistryChinese Academy of Sciences27 South Taoyuan RoadTaiyuan030001China center of Materials Science and Optoelectronics engineering University of Chinese Academy of SciencesBeijing100049China Department of chemistry and chemical engineering Taiyuan Institute of TechnologyTaiyuanShanxi030008China Beijing Key Laboratory of Fuels Cleaning and advanced catalytic Emission Reduction Technology/college of New Materials and chemical engineering Beijing Institute of Petrochemical TechnologyBeijing102617China

Melamine formaldehyde foam(MFF)generates many poisonous chemicals through the traditional recycling methods for organic resin ***,a high MFF degradation ratio of ca.97 wt.%was achieved under the mild conditions(160℃)in a NaOH–H2O system with ammelide and ammeline as the main degradation *** alkaline solvent had an obvious corrosion effect for MFF,as indicated by scanning electron microscopy(SEM).The reaction process and products distribution were studied by Fourier-transform infrared spectroscopy(FTIR),X-ray photoelectron spectroscopy(XPS),and ^(13)C nuclear magnetic resonance(NMR).Besides,the MFF degradation products that have the similar chemical structures and bonding performances to those of melamine can be directly used as the raw material for synthesis of melamine urea-formaldehyde resins(MUFs).Moreover,the degradation system demonstrated here showed the high degradation efﬁciency after reusing for 7 *** degradation process generated few harmful pollutants and no pre-or post-treatments were required,which proves its feasibility in the safe removal or recovery of waste MFF.

关键词： Melamine formaldehyde foam Degradation Alkaline hydrolysis Recycling

An Efficient Multifunctional Soluble Catalyst for Li-O_(2) Batteries

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CCS chemistry 2024年第7期6卷 1810-1820页

作者： Shuochao Xing Zhengcai Zhang Yaying Dou Minghui Li Jing Wu Zhang Zhang Zhen Zhou Interdisciplinary research center for Sustainable Energy Science and engineering(IRC4SE2) School of Chemical EngineeringZhengzhou UniversityZhengzhou 450001 Key Laboratory of advanced Energy Materials chemistry Ministry of EducationCollege of ChemistryNankai UniversityTianjin 300071

Aprotic lithium-oxygen(Li-O_(2))batteries have a high theoretical energy density,but they face challenges such as cathode blockage,high charge overpotential,and poor cycling *** are caused by sluggish reaction kinetics and severe parasitic *** the performance of Li-O_(2) batteries necessitates the development of efficient *** catalysts not only augment both the oxygen reduction reaction(ORR)and the oxygen evolution reaction(OER)but also inhibit undesirable parasitic *** this work,we demonstrated for the first time a multifunctional soluble catalyst of iridium(III)acetylacetonate(Ir(acac)_(3))that could speed up oxygen ***(acac)_(3) regulated the ORR pathway and the reactivity of superoxide radical species by forming a reversible intermediate complex(Ir(acac)_(3)-O_(2)^(−)).During charging,Ir(acac)_(3) acted as a redox mediator and aided in Li_(2)O_(2) decomposition by reacting with superoxide ***,as demonstrated by operando UV-visible spectroscopy,the lower charge potential significantly reduced the generation of highly reactive singlet oxygen(^(1)O_(2))*** a result,the Ir(acac)_(3)-mediated Li-O_(2) battery showed low overpotential,large capacity,and stable *** study offers a new approach to achieving efficient Li-O_(2) batteries and provides an opportunity to suppress parasitic reactions.

关键词： Li-O_(2)battery soluble catalyst superoxide species organometallics singlet oxygen

Mechanism of interfacial effects in sodium-ion storage devices

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Nano research 2024年第3期17卷 1313-1326页

作者： Yifan Wei Lingxing Zan Huicong Xia Wenfu Yan Jia-Nan Zhang college of Materials Science and engineering Zhengzhou UniversityZhengzhou 450001China Key Laboratory of advanced Energy catalytic and Functional Material Preparation of Zhengzhou City Zhengzhou 450001China Key Laboratory of chemical Reaction engineering of Shaanxi Province College of Chemistry&Chemical EngineeringYan’an UniversityYan’an 716000China State Key Laboratory of Inorganic Synthesis and Preparative chemistry and college of chemistry Jilin UniversityChangchun 130012China

Rechargeable sodium-ion batteries(SIBs)are considered as the next-generation secondary *** performance of SIB is determined by the behavior of its electrode surface and the electrode–electrolyte interface during charging and ***,the characteristics of these surfaces and interfaces should be analyzed to realize large-scale energy storage systems with high energy density and long-cycle *** various studies have investigated the properties of electrode materials,few studies have focused on the construction of stable and efficient SIB interfaces,and even fewer have explored the mechanisms of interfacial effects;however,the strategies of regulating interfacial effects are yet to be completely ***,the results obtained thus far are insufficient to draw systematic *** present study reviews the literature on the mechanism of interfacial effects in Na+storage *** interfaces in a sodium-ion storage device include a heterogeneous interface between electrode materials,a solid electrolyte interphase,and a cathode electrolyte *** interfacial effects during the intercalation,transformation,and alloy reactions and the resulting overall battery performance were theoretically *** this review,we aim to provide a theoretical basis for optimizing the structures of electrode surface and electrode–electrolyte interface to optimize the performance of *** addition,the challenges of investigating interfacial effects and several possible helpful methods and opportunities for studying the mechanisms of interfacial effects in SIBs will be presented.

关键词： sodium-ion storage interfacial effects solid electrolyte interphase cathode electrolyte interphase