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Journal of Magnesium and Alloys 2024年第1期12卷 110-119页

作者： Man-Fai Ng Kai Xiang Kuah Teck Leong Tan Daniel John Blackwood Department of Materials Science&Engineering National University of Singapore9 Engineering Drive 1Singapore 117575Republic of Singapore Institute of High Performance Computing(IHPC) Agency for ScienceTechnology and Research(A∗STAR)1 Fusionopolis Way#16-16 ConnexisSingapore 138632Republic of Singapore

The corrosion rates of additive-manufactured Mg alloys are higher than their as-cast counterparts,possibly due to increased kinetics for the hydrogen evolution reaction on secondary phases,which may include oxide *** Kelvin Probe Force Microscopy demonstrated that MgO inclusions could act as cathodes for Mg corrosion,but their low conductivity likely precludes ***,the density of state calculations through density functional theory using hybrid HSE06 functional revealed overlapping electronic states at the Mg/MgO interface,which facilitates electron transfers and participates in redox *** determination of the hydrogen absorption energy at the Mg/MgO interface reveals it to be an excellent catalytic site,with HER being found to be a factor of 23x more efficient at the interface than on metallic *** results not only support the plausibility of the Mg/MgO interface being an effective cathode to the adjacent anodic Mg matrix during corrosion but also contribute to the understanding of the enhanced cathodic activities observed during the anodic dissolution of magnesium.

关键词： Magnesium Magnesium oxide Interface hydrogen evolution DFT

Key role of electron accessibility at the noble metal-free catalytic interface in hydrogen evolution reaction

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Nano Research 2024年第4期17卷 2538-2545页

作者： Dongchen Han Nanxing Gao Yuyi Chu Zhaoping Shi Ying Wang Junjie Ge Meiling Xiao Changpeng Liu Wei Xing 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 Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Jilin Province Key Laboratory of Low Carbon Chemical Power Sources Changchun 130022China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The reactant concentration at the catalytic interface holds the key to the activity of electrocatalytic hydrogen evolution reaction(HER),mainly referring to the capacity of adsorbing hydrogen and electron *** hydrogen adsorption free energy(ΔGH)as a reactivity descriptor,the volcano curve based on Sabatier principle is established to evaluate the hydrogen evolution activity of ***,the role of electron as reactant received insufficient attention,especially for noble metal-free compound catalysts with poor conductivity,leading to cognitive gap between electronic conductivity and apparent catalytic *** we successfully construct a series of catalyst models with gradient conductivities by regulating molybdenum disulfide(MoS_(2))electronic bandgap via a simple solvothermal *** demonstrate that the conductivity of catalysts greatly affects the overall catalytic *** further elucidate the key role of intrinsic conductivity of catalyst towards water electrolysis,mainly concentrating on the electron transport from electrode to catalyst,the electron accumulation process at the catalyst layer,and the charge transfer progress from catalyst to *** and experimental evidence demonstrates that,with the enhancement in electron accessibility at the catalytic interface,the dominant parameter governing overall HER activity gradually converts from electron accessibility to combination of electron accessibility and hydrogen adsorbing *** results provide the insight from various perspective for developing noble metal-free catalysts in electrocatalysis beyond HER.

关键词： conductivity molybdenum disulfide catalytic interface electron accessibility hydrogen evolution charge transfer.

Molecular solid solution of lanthanide-titanium-oxo clusters with enhanced photocatalytic hydrogen evolution

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Science China Chemistry 2024年第2期67卷 529-535页

作者： Rong Chen Chao-Long Chen Hui Zhang Zi-Han Wang Fu-Li Sun Ming-Hao Du Gui-Lin Zhuang Cheng Wang La-Sheng Long Lan-Sun Zheng Xiang-Jian Kong Collaborative Innovation Centre of Chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surfaces and Department of Chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China College of Chemical Engineering Zhejiang University of TechnologyHangzhou310032China

Molecular solid solutions of metal clusters containing different metal centers with well-defined structures can accurately regulate the HOMO-LUMO gap,but are rarely ***,a series of colorless lanthanide-titanium-oxo clusters Ln_(2)Ti_4(μ_(2)-O)_(2)(μ_(3)-O)_4(Piv)_(10)(THF)_(2)(Ln_(2)Ti_4,Ln = Eu,Gd,Tb,and Ce,HPiv = pivalic acid) were synthesized by the reaction of pivalic acid with Ln(Ac)_(3) and titanium *** light yellow crystal of cluster solid solutions Eu_(2)Ti_(4-x)Cd_(x),containing a mixture of Eu_(2)Ti_4 and Eu_(2)Ti_(3)Cd,was obtained by in situ doping Cd^(2+) and S^(2–).Eu_(2)Ti_(3.92)Cd_(0.08) displays efficient photocatalytic hydrogen evolution activity without a co-catalyst,which is up to 2.6 times that of Eu_(2)Ti_*** time-resolved transient absorption spectroscopy and spin-polarized density functional calculations showed that the enhanced photocatalytic performance of Eu_(2)Ti_(4-x)Cd_(x) can be attributed to the narrower HOMO-LUMO gap and lower LUMO position than that of Eu_(2)Ti_*** studyprovides an in situ doping method to realize the simple preparation of cluster solid solution.

关键词： molecular solid solution lanthanide-titanium-oxo clusters photocatalytic hydrogen evolution

Photoelectrocatalytic hydrogen evolution and synchronous degradation of organic pollutants by pg-C_(3)N_(4)/β-FeOOH S-scheme heterojunction

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Science China(Technological Sciences) 2024年第4期67卷 1238-1252页

作者： LI XiBao HAN Tao ZHOU YingTang XIE Yu LUO YiDan HUANG JunTong CHEN Zhi DENG Fang School of Materials Science and Engineering Nanchang Hangkong UniversityNanchang 330063China National-Local Joint Engineering Research Center of Heavy Metal Pollutants Control and Resource Utilization Nanchang Hangkong UniversityNanchang 330063China Zhejiang Key Laboratory of Petrochemical Environmental Pollution Control National Engineering Research Center for Marine AquacultureMarine Science and Technology CollegeZhejiang Ocean UniversityZhoushan 316022China

Crafting photoelectrocatalytic materials with robust oxidation-reduction properties for simultaneous hydrogen evolution and pollutant degradation poses a formidable *** this study,a pg-C_(3)N_(4)/β-FeOOH S-scheme heterostructure with a special energy band structure was developed by anchoring porous pg-C_(3)N_(4)on needle shapedβ-*** as a hole extraction layer,needle-leaf-likeβ-FeOOH can facilitate efficient hole migration and enhance charge ***,the optimized 0.2-pg-C_(3)N_(4)/β-FeOOH could degrade 78%of ofloxacin(OFLO)in 90 *** organic pollutants could absorb a large number of holes,which prompted a greater proportion of photogenerated electrons to actively participate in the hydrogen evolution reaction at the ***,the hydrogen production of 0.2-pg-C_(3)N_(4)/β-FeOOH reached 1452.88μmol cm^(-2)h^(-1),exhibiting a notable increase of 61.81-165.12μmol cm^(-2)h^(-1)compared with that in the absence of *** and theoretical calculation results underscore that this investigation is grounded in a distinctive electron and hole dual channel transfer *** findings offer novel insights for the future development of S-scheme heterojunction photoelectrocatalytic materials capable of concurrently degrading pollutants and promoting hydrogen evolution.

关键词： photoelectrocatalysis hydrogen evolution degradation synchronous S-scheme heterojunction

Atomically precise Ru-O-Ru clusters for enhanced water dissociation in alkaline hydrogen evolution

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Nano Research 2024年第8期17卷 6993-7000页

作者： Dong Liu Li Xu Sicheng Li Airong Xu Yuanhua Sun Tong Liu Mengyuan Liu Huijuan Wang Xiaokang Liu Tao Yao Tao Ding Hefei National Research Center for Physical Sciences at the Microscale School of Nuclear Science and TechnologyKey Laboratory of Precision and Intelligent ChemistryNational Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230029China Experimental Center of Engineering and Materials Science University of Science and Technology of ChinaHefei 230026China

Atomic clusters typically exhibit distinctive electronic structures and physicochemical ***,as the size decreases,their ability to adsorb and dissociate water also diminishes,thereby affecting chemical reactions involving water *** the adsorption and dissociation capabilities of atomic clusters towards water molecules and elucidating the mechanisms underlying their performance enhancement have become important research ***,employing the carrier-anchored strategy,Ru-O-Ru atomic clusters were prepared and displayed excellent activity and durability in the hydrogen evolution ***,the Ru-O-Ru atomic clusters exhibited only 86 mV overpotential at 100 mA·cm−^(2) and superior membrane-electrode-assembly activity than commercial Ru/C *** radiation-based Fourier transform infrared spectroscopic measurements revealed that the modification of oxygen in Ru-O-Ru units promoted the reorientation of water molecules from a H-up orientation to H-down,therefore,enhanced the formation of strong hydrogen-bond network of interfacial water on the surface of Ru-O-Ru clusters,leading to enhanced adsorption and dissociation of water and accelerated Volmer *** findings provide a potential strategy and deep insights for the development of atomic clusters in electrocatalysts.

关键词： hydrogen evolution in-situ Fourier transform infrared(FTIR) Ru catalysts electrocatalysis atomic clusters

Enhancing hydrogen evolution and oxidation kinetics through oxygen insertion into nickel lattice

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Journal of Energy Chemistry 2024年第8期95卷 529-539,I0012页

作者： Wanli Liang Xiyu Gong Jinchang Xu Zixuan Dan Fanyan Xie Hulei Yu Hao-Fan Wang Yanshuo Jin Hongjuan Wang Yonghai Cao Hui Meng Hao Yu School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou 510641GuangdongChina Siyuan Laboratory Guangzhou Key Laboratory of Vacuum Coating Technologies and New Energy MaterialsGuangdong Provincial Engineering Technology Research Center of Vacuum Coating Technologies and New Energy MaterialsGuangdong Provincial Key Laboratory of Optical Fiber Sensing and CommunicationsDepartment of PhysicsJinan UniversityGuangzhou 510632GuangdongChina GBA Branch of Aerospace Information Research Institute Chinese Academy of SciencesGuangzhou 510700GuangdongChina Instrumental Analysis&Research Center Sun Yat-sen UniversityGuangzhou 510275GuangdongChina School of Materials Science and Engineering South China University of TechnologyGuangzhou 510641GuangdongChina

Nickel-based materials,including metallic Ni and Ni oxide,have been widely studied in the exploration of non-precious-metal hydrogen electrocatalysts,but neither pure Ni nor NiO is ideal for the hydrogen evolution reaction(HER)and hydrogen oxidation reaction(HOR).In this paper,an oxygen insertion strategy was applied on nickel to regulate its hydrogen electrocatalytic performance,and the oxygen-inserted nickel catalyst was successfully obtained with the assistance of tungsten dioxide support(denoted as O-Ni/WO_(2)).The partial insertion of oxygen in Ni maintains the face-centered cubic arrangement of Ni atoms,simultaneously expanding the lattice and increasing the lattice ***,the adsorption strength of^(*)H and^(*)OH on Ni is optimized,thus resulting in superior electrocatalytic performance of0-Ni/WO_(2)in alkaline HER/*** Tafel slope of O-Ni/WO_(2)@NF for HER is 56 mV dec^(-1),and the kinetic current density of O-Ni/WO_(2)for HOR reaches 4.85 mA cm^(-2),which is ahead of most currently reported *** proposed strategy of inserting an appropriate amount of anions into the metal lattice could provide more possibilities for the design of high-performance catalysts.

关键词： hydrogen evolution hydrogen oxidation Nickel Oxygen insertion Adsorption free energy

Data-driven rational design of single-atom materials for hydrogen evolution and sensing

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Nano Research 2024年第4期17卷 3352-3358页

作者： Lei Zhou Pengfei Tian Bowei Zhang Fu-Zhen Xuan Shanghai Key Laboratory of Intelligent Sensing and Detection Technology East China University of Science and TechnologyShanghai 200237China School of Mechanical and Power Engineering East China University of Science and TechnologyShanghai 200237China Key Laboratory of Pressure Systems and Safety of Ministry of Education East China University of Science and TechnologyShanghai 200237China

Herein we proposed a data-driven high-throughput principle to screen high-performance single-atom materials for hydrogen evolution reaction(HER)and hydrogen sensing by combing the theoretical computations and a topology-based multi-scale convolution kernel machine learning *** the rational training by 25 groups of data and prediction of all 168 groups of single-atom materials for HER and sensing,respectively,a high prediction accuracy(>0.931 R^(2) score)was achieved by our *** show that the promising HER catalysts include Pt atoms in C_(4) and Sc atoms in C_(1)N_(3) coordination ***,Y atoms in C_(4) coordination environment and Cd atoms in C_(2)N_(2)-ortho coordination environment were predicted with great potential as hydrogen sensing *** method provides a way to accelerate the discovery of innovative materials by avoiding the time-consuming empirical principles in experiments.

关键词： machine learning single-atom materials sensing hydrogen evolution

Function-reversible facets enabling SrTiO_(3)nanocrystals for improved photocatalytic hydrogen evolution

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Frontiers in Energy 2024年第1期18卷 101-109页

作者： Bin WANG Bei AN Xiaoqian LI Shaohua SHEN School of Physics Key Laboratory for Non-equilibrium Synthesis and Modulation of Condensed Matter(Ministry of Education)Key Laboratory of Shaanxi for Advanced Materials and Mesoscopic PhysicsXi’an Jiaotong UniversityXi’an 710049China International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power EngineeringXi’an Jiaotong UniversityXi’an 710049China

It has been widely reported that,for faceted nanocrystals,the two adjacent facets with different band levels contribute to promoted charge separation,and provide active sites for photocatalytic reduction and oxidation reaction,*** such cases,only one family of facets can be used for photocatalytic hydrogen ***,by using SrTiO_(3)nanocrystals enclosed by{023}and{001}facets as a model photocatalyst,this paper proposed a strategy to achieve the full-facets-utilization of the nanocrystals for photocatalytic hydrogen via chemically depositing Pt nanoparticles on all *** photo-deposition experiment of CdS provided direct evidence to demonstrate that the{023}facets which were responsible for photooxidation reaction can be function-reversed for photocatalytic hydrogen evolution after depositing Pt nanoparticles,together with the{001}***,the full-facets-utilization led to a much-improved activity for photocatalytic hydrogen,in contrast to those SrTiO_(3)nanocrystals with only{001}facets deposited by Pt nanoparticles via a photo-deposition method.

关键词： SrTiO_(3)nanocrystals crystal facets photocatalysis hydrogen evolution

Orientation controlled photogenerated carriers on selfsupporting CdS/Ni_(3)S_(2) paper toward photocatalytic hydrogen evolution and biomass upgrading

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Rare Metals 2024年第5期43卷 2015-2025页

作者： Xiao-Yan Liu Qing Cao Gui-Xiang Li Hui Liu Li-Li Zeng Li-Li Zhao Bin Chang Xi-Wen Wang Hong Liu Wei-Jia Zhou Institute for Advanced Interdisciplinary Research School of Chemistry and Chemical EngineeringUniversity of JinanJinan 250022China Institute of Chemical Sciences and Engineering Ecole Polytechnique Federale de Lausanne1015LausanneSwitzerland KAUST Catalysis Center King Abdullah University of Science and TechnologyThuwal 23955-6900Kingdom of Saudi Arabia School of Environment and Energy South China University of TechnologyGuangzhou Higher Education Mega CenterGuangzhou 510006China State Key Laboratory of Crystal Materials Shandong UniversityJinan250100China School of Mechanical Engineering Xi'an Jiaotong UniversityXi'an 710054China

The appropriate regulation of band structure is an effective strategy in constructing efficient photocatalytic *** photocatalytic system mainly employs powder photocatalysts,which makes their recovery reliant on expensive separation processes and severely limits their industrial ***,we constructed a novel CdS/Ni_(3)S_(2)heterostructure using free-standing and flexible nickel fiber paper as the *** regulated energy band structure achieves effective electron–hole *** as-synthesized flexible photocatalyst exhibits considerable photocatalytic activity toward the H_(2)evolution reaction under visible-light irradiation,with an H_(2)production rate of5.63μmol·cm^(-2)·h^(-1)(14.1 mmol·g^(-1)cat·h^(-1)according to the catalyst loading content).Additionally,the otherwisewasted excited holes simultaneously drive organic transformations to yield value-added organic products,thus markedly improving the photocatalytic H_(2)evolution *** a photocatalytic system is scaled up further,where a self-supported 20 cm×25 cm sample achieves a champion H_(2)production rate of 60-80μmol·h^(-1)under practical sun *** newly developed self-supported photocatalyst produces opportunities for practical solar H2production with biomass upgrading.

关键词： Self-supporting photocatalyst CdS/Ni_(3)S_(2) heterojunction hydrogen evolution Biomass upgrading Large-scaleapplication

Designing multi-heterogeneous interfaces of Ni-MoS_(2)@NiS_(2)@Ni_(3)S_(2)hybrid for hydrogen evolution

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Nano Research 2024年第6期17卷 4782-4789页

作者： Haoxuan Yu Junan Pan Yuxin Zhang Longlu Wang Huachao Ji Keyu Xu Ting Zhi Zechao Zhuang College of Electronic and Optical Engineering&College of Flexible Electronics(Future Technology) Nanjing University of Posts&Telecommunications(NJUPT)Nanjing 210023China Department of Chemical Engineering Columbia UniversityNew YorkNY 10027USA

The transition metal chalcogenides represented by MoS_(2)are the ideal choice for non-precious metal-based hydrogen evolution ***,whether in acidic or alkaline environments,the catalytic activity of pure MoS_(2)is still difficult to compete with *** studies have shown that the electronic structure of materials can be adjusted by constructing lattice-matched heterojunctions,thus optimizing the adsorption free energy of intermediates in the catalytic hydrogen production process of materials,so as to effectively improve the electrocatalytic hydrogen production activity of ***,it is still a great challenge to prepare heterojunctions with lattice-matched structures as efficient electrocatalytic hydrogen production ***,we developed a one-step hydrothermal method to construct Ni-MoS_(2)@NiS_(2)@Ni_(3)S_(2)(Ni-MoS_(2)on behalf of Ni doping MoS_(2))electrocatalyst with multiple heterogeneous interfaces which possesses rich catalytic reaction *** Ni-MoS_(2)@NiS_(2)@Ni_(3)S_(2)electrocatalyst produced an extremely low overpotential of 69.4 mV with 10 mA·cm^(−2)current density for hydrogen evolution reaction(HER)in 1.0 M *** work provides valuable enlightenment for exploring the mechanism of HER enhancement to optimize the surface electronic structure of MoS_(2),and provides an effective idea for constructing rare metal catalysts in HER and other fields.

关键词： MoS_(2) heterojunctions multiple heterogeneous interfaces hydrogen evolution