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Mechanistic insight into the synergy between nickel single atoms and nanoparticles on N-doped carbon for electroreduction of CO2

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Journal of Energy Chemistry 2025年第1期100卷 327-336页

作者： Mingdong Sun Wenwen Guan Cailing Chen Chao Wu Xiaoling Liu Biao Meng Tao Chen Yu Han Jun Wang Shibo Xi Yu Zhou State Key Laboratory of materials-Oriented Chemical Engineering College of Chemical Engineering Nanjing Tech University Advanced Membranes and Porous materials Center Physical Sciences and Engineering Division King Abdullah University of Science and Technology Institute of Sustainability for Chemicals Energy and Environment A*STAR (Agency for Science Technology and Research) College of materials Science and Engineering Sichuan University

The synergy of single atoms （SAs） and nanoparticles （NPs） has demonstrated great potential in promoting the electrocatalytic carbon dioxide reduction reaction （CO2RR）;however,the rationalization of the SAs/NPs proportion remains one challenge for the catalyst ***,a Ni2+-loaded porous poly（ionic liquids）(PIL) precursor synthesized through the free radical self-polymerization of the ionic liquid monomer,1-allyl-3-vinylimidazolium chloride,was pyrolyzed to prepare the Ni,N co-doped carbon materials,in which the proportion of Ni SAs and NPs could be facilely modulated by controlling the annealing *** catalyst Ni-NC-1000 with a moderate proportion of Ni SAs and NPs exhibited high efficiency in the electrocatalytic conversion of CO2into *** Ni K-edge X-ray absorption near-edge structure （XANES） spectra and theoretical calculations were conducted to gain insight into the synergy of Ni SAs and *** charge transfer from Ni NPs to the surrounding carbon layer and then to the Ni SAs resulted in the electron-enriched Ni SAs active *** the electroreduction of CO2,the coexistence of Ni SAs and NPs strengthened the CO2activation and the affinity towards the key intermediate of*COOH,lowering the free energy for the potential-determining*CO2→*COOH step,and therefore promoted the catalysis efficiency.

关键词： Single atom catalyst Synergy effect Carbon catalyst Electrocatalysis

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“Zero‑Strain” NiNb_(2)O_(6) Fibers for All‑Climate Lithium Storage

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Nano-Micro Letters 2025年第1期17卷 348-360页

作者： Yan Zhao Qiang Yuan Liting Yang Guisheng Liang Yifeng Cheng Limin Wu Chunfu Lin Renchao Che College of Physics Donghua UniversityShanghai 201620People’s Republic of China School of materials Science and Engineering Institute of Materials for Energy and EnvironmentQingdao UniversityQingdao 266071People’s Republic of China Laboratory of Advanced materials Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsAcademy for Engineering&TechnologyFudan UniversityShanghai 200438People’s Republic of China Zhejiang Laboratory Hangzhou 311100People’s Republic of China Inner Mongolia University Hohhot 010021People’s Republic of China

Niobates are promising all-climate Li^(+)-storage anode material due to their fast charge transport,large specific capacities,and resistance to electrolyte ***,their moderate unit-cellvolume expansion(generally 5%–10%)during Li^(+)storage causes unsatisfactory long-term ***,“zero-strain”NiNb_(2)O_(6) fibers are explored as a new anode material with comprehensively good electrochemical *** Li^(+)storage,the expansion of electrochemical inactive NiO_(6) octahedra almost fully offsets the shrinkage of active NbO_(6) octahedra through reversible O *** superior volume-accommodation capability of the NiO_(6) layers guarantees the“zero-strain”behavior of NiNb_(2)O_(6) in a broad temperature range(0.53%//0.51%//0.74%at 25//−10//60℃),leading to the excellent cyclability of the NiNb_(2)O_(6) fibers(92.8%//99.2%//91.1%capacity retention after 1000//2000//1000 cycles at 10C and 25//−10//60℃).This NiNb_(2)O_(6) material further exhibits a large reversible capacity(300//184//318 mAh g−1 at 0.1C and 25//−10//60℃)and outstanding rate performance(10 to 0.5C capacity percentage of 64.3%//50.0%//65.4%at 25//−10//60℃).Therefore,the NiNb_(2)O_(6) fibers are especially suitable for large-capacity,fast-charging,long-life,and all-climate lithium-ion batteries.

关键词： NiNb_(2)O_(6)porous fiber “Zero-strain”mechanism Electrochemical property Harsh-temperature operation Operando characterization

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Overview of in-situ oxygen production technologies for lunar resources

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International Journal of Minerals,Metallurgy and materials 2025年第2期32卷 233-255页

作者： Youpeng Xu Sheng Pang Liangwei Cong Guoyu Qian Dong Wang Laishi Li Yusheng Wu Zhi Wang College of materials Science and Engineering Shenyang University of TechnologyShenyang 110870China CAS Key Laboratory of Green process and Engineering National Engineering Research Center for Green Recycling of Strategic Metal ResourcesInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China Innovation Academy for Green Manufacture Chinese Academy of SciencesBeijing 100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China

The rich resources and unique environment of the Moon make it an ideal location for human expansion and the utilization of extraterrestrial ***,crucial for supporting human life on the Moon,can be extracted from lunar regolith,which is highly rich in oxygen and contains polymetallic *** oxygen and metal extraction can be achieved using existing metallurgical ***,the ample reserves of water ice on the Moon offer another means for oxygen *** paper offers a detailed overview of the leading technologies for achieving oxygen production on the Moon,drawing from an analysis of lunar resources and environmental *** delves into the principles,processes,advantages,and drawbacks of water-ice electrolysis,two-step oxygen production from lunar regolith,and one-step oxygen production from lunar *** two-step methods involve hydrogen reduction,carbothermal reduction,and hydrometallurgy,while the one-step methods encompass fluorination/chlorination,high-temperature decomposition,molten salt electrolysis,and molten regolith electrolysis(MOE).Following a thorough comparison of raw materials,equipment,technology,and economic viability,MOE is identified as the most promising approach for future in-situ oxygen production on the *** the corrosion characteristics of molten lunar regolith at high temperatures,along with the Moon's low-gravity environment,the development of inexpensive and stable inert anodes and electrolysis devices that can easily collect oxygen is critical for promoting MOE technology on the *** review significantly contributes to our understanding of in-situ oxygen production technologies on the Moon and supports upcoming lunar exploration initiatives.

关键词： lunar resources in-situ oxygen production space metallurgy molten lunar regolith electrolysis

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Construction of Ni single-atom coordinated with doped N and S elements for mild hydrogenation of methyl acrylate to methyl propionate

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Nano Research 2025年第1期18卷 217-224页

作者： Taolue Sun Chen Jian Gang Wang Hui Zhao Guoliang Zhang Zengxi Li Chunshan Li State Key Laboratory of Mesoscience and Engineering CAS Key Laboratory of Green Process and EngineeringBeijing Key Laboratory of Ionic Liquids Clean ProcessInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China Huizhou Institute of Green Energy and Advanced materials Huizhou 516081China Advanced Energy Science and Technology Guangdong Laboratory Huizhou 516081China

Although the nickel-based catalyst is able toexhibit comparative catalytic activity to noble metal formethyl acrylate hydrogenation,it requires strict reactioncondition,which can be improved by regulation ofcoordination *** this study,we constructed akind of Ni single-atom coordinated with N and S(Ni-NSC)through the pyrolysis of organic Ni-based precursors at600℃.The existence and fine structure of Ni single-atom were confirmed by the spherical electron microscopicobservation in combination with the X-ray absorption spectroscopy(XAS)*** addition,the catalytichydrogenation assessment suggested that the as-prepared Ni-NSC catalyst exhibited higher activity and stability than theNi/NSC supported catalyst prepared by incipient wetness impregnation *** remarkable catalytic activity was dueto the high dispersion and density of Ni single-atom and weak adsorption energy of intermediates on these Ni sites.

关键词： methyl acrylate mild hydrogenation Ni single-atom coordination environment adsorption energy

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Atomically precise nickel-sulfur clusters for efficient electrochemical 2,5-hydroxymethylfurfural oxidation

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Nano Research 2025年第1期18卷 140-148页

作者： Fen Wang Lu-Yu Liu Sha-Sha Cui Ting-Ting Li Xiao-Meng Yang Zhijuan Liu Yanyong Wang Henan Key Laboratory of Crystalline Molecular Functional materials Henan International Joint Laboratory of Tumor Theranostical Cluster MaterialsGreen Catalysis Centerand College of ChemistryZhengzhou UniversityZhengzhou 450001China State Key Laboratory of Chem/Bio-sensing and Chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China

Nickel sulfide exhibits excellent catalytic activity in the electrochemical 2,5-hydroxymethylfurfural oxidation reaction(HMFOR).However,due to the polydispersity of nanoparticles,it is difficult to establish a clear structure-activity relationship at the atomic *** this work,we have successfully synthesized atomically precise Ni_(6)(PET)_(12)and Ni_(4)(PET)_(8)clusters(PET:2-phenylethanethiol)for ***^(2+)and S_(2)-with atomic ratio of 1:2 was mainly existed in Ni_(6)(PET)_(12)and Ni_(4)(PET)_(8)to form Ni-S *** electrochemical test results have suggested both Ni_(6)(PET)_(12)and Ni_(4)(PET)_(8)displayed outstanding electrocatalytic ability for *** Ni_(6)(PET)_(12)exhibited better electrocatalytic ability than Ni_(4)(PET)_(8)with higher current density,lower overpotential and faster reaction *** superior electrochemical ability of Ni_(6)(PET)_(12)may be due to the enhanced adsorption towards HMF molecule with strong interaction towards hydroxyl group and furan ***,it found that the Ni^(2+)species in Ni_(6)(PET)_(12)could rapidly oxidized into Ni^(3+)species,which could spontaneously capture electron and proton from HMF for *** theoretical calculation demonstrated that the Ni_(6)(PET)_(12)process lower free energy barrier than Ni_(4)(PET)_(8)to display excellent electrocatalytic *** work is of great significance for designing efficient electrocatalysts for HMFOR.

关键词： atomically precise nickel nanoclusters 2 5-hydroxymethylfurfural electro-oxidation Ni3+species

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Boosting hydrocarbon conversion via Cu-doping induced oxygen vacancies on CeO2 in CO2 electroreduction

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Journal of Energy Chemistry 2025年第1期100卷 66-76页

作者： Lei Xue Tong Shi Chenhui Han Heng Zhang Fenrong Liu Haorun Li Yan Wang Xiaojun Gu Shanghong Zeng Inner Mongolia Key Laboratory of Chemistry and Physics of Rare Earth materials School of Chemistry and Chemical Engineering Inner Mongolia University State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences Institute of catalysis Department of Chemistry Zhejiang University National Key Laboratory of Baiyunobo Rare Earth Resource Research and Comprehensive Utilization Baotou Research Institute of Rare Earths

Conversion of CO2back to hydrocarbons is the most direct way of closing the“carbon cycle”,and its significance is further enlarged if this process is driven by renewable energies such as ***,precisely controlling the product selectivity towards hydrocarbons against the competitive hydrogen evolution remains challenging,especially for Cu-based ***,we report a novel defect engineering strategy,by which Cu-doping-induced oxygen vacancies on CeO2nanorods were effectively created,with adjustable vacancy/Cu *** resulting optimum catalyst shows up to 79% catalytic current density to hydrocarbons （excluding CO）,with 49% faradaic efficiency to *** and density functional theory unveil that the ratio between oxygen vacancy and Cu affects significantly the formation of*CHO and activation of H2O,which leads to the following deep hydrogenation to *** findings may spur new insights for designing and developing more controllable chemical process relevant to CO2utilization.

关键词： Oxygen vacancy Hydrocarbon production Reaction mechanism

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Designing Electronic Structures of Multiscale Helical Converters for Tailored Ultrabroad Electromagnetic Absorption

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Nano-Micro Letters 2025年第1期17卷 439-455页

作者： Zhaobo Feng Chongbo Liu Xin Li Guangsheng Luo Naixin Zhai ruizhe Hu Jing Lin Jinbin Peng Yuhui Peng Renchao Che Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle School of Environmental and Chemical EngineeringNanchang Hangkong UniversityNanchang 330063People’s Republic of China School of Physics and materials Nanchang UniversityNanchang 330031People’s Republic of China Key Laboratory of Nondestructive Testing Ministry of EducationNanchang Hangkong UniversityNanchang 330063People’s Republic of China Laboratory of Advanced materials Shanghai Key Lab of Molecular Catalysis and Innovative MaterialsAcademy for Engineering and TechnologyFudan UniversityShanghai 200438People’s Republic of China

Atomic-scale doping strategies and structure design play pivotal roles in tailoring the electronic structure and physicochemical property of electromagnetic wave absorption(EMWA)***,the relationship between configuration and electromagnetic(EM)loss mechanism has remained ***,drawing inspiration from the DNA transcription process,we report the successful synthesis of novel in situ Mn/N co-doped helical carbon nanotubes with ultrabroad EMWA *** calculation and EM simulation confirm that the orbital coupling and spin polarization of the Mn–N4–C configuration,along with cross polarization generated by the helical structure,endow the helical converters with enhanced EM *** a result,HMC-8 demonstrates outstanding EMWA performance,achieving a minimum reflection loss of−63.13 dB at an ultralow thickness of 1.29 *** precise tuning of the graphite domain size,HMC-7 achieves an effective absorption bandwidth(EAB)of 6.08 GHz at 2.02 mm ***,constructing macroscale gradient metamaterials enables an ultrabroadband EAB of 12.16 GHz at a thickness of only 5.00 mm,with the maximum radar cross section reduction value reaching 36.4 dB *** innovative approach not only advances the understanding of metal–nonmetal co-doping but also realizes broadband EMWA,thus contributing to the development of EMWA mechanisms and applications.

关键词： Metal-nonmetal co-doping 3d-2p orbital coupling Spin polarization Helical structure Broadband EM wave absorption

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Electrochemical conversion of methane to bridge the gap in the artificial carbon cycle

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Journal of Energy Chemistry 2025年第1期100卷 286-308页

作者： Yuhao Peng Yuefeng Song Ihar Razanau Juanxiu Xiao Wei Xiao Di Hu Guoxiong Wang College of Chemistry and Molecular Sciences Hubei Key Laboratory of Electrochemical Power Sources Wuhan University State Key Laboratory of catalysis Dalian National Laboratory for Clean Energy iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Dalian Institute of Chemical Physics Chinese Academy of Sciences Laboratory of Physical-Chemical Technologies SSPA Scientific and Practical Materials Research Centre of NAS of Belarus State Key Laboratory of Marine Resources Utilization in South China Sea Collaborative Innovation Center of Marine Science and Technology School of Marine Science and Engineering Hainan University Department of Chemical and environmental Engineering University of Nottingham Ningbo China

Methane, an abundant one-carbon（C1） resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO2emissions and coke deposition. Electrochemical conversion of methane（ECM） using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO2emission.

关键词： Methane Electrochemical conversion Reaction mechanism Catalyst design Electrode Electrocatalysis

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Comparative Study of the Structure and Properties of Ti—O-based Nanowire Films Prepared by Anodization and Chemical Oxidation Methods

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Journal of materials Science & Technology 2014年第9期30卷 878-883页

作者： Xinwen Huang Zongjian Liu Resource & environment catalysis Institute College of Chemical Engineering and Materials ScienceZhejiang University of Technology College of Biological and environmental Engineering Zhejiang University of Technology

Net-like titanium oxide or H-titanate nanowire films were grown on Ti substrates in 2 mol/L NaOH solutions at 80 ℃ via anodization method or chemical oxidation followed by proton-exchange. The microstructure, thermal stability and photoelectrochemical property of two types of films were investigated by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, and photocurrent measurement. It is found that the anodic film mainly consists of a 500-nm-thick nenowire layer whereas the film formed by chemical oxidization is made up of two layers： a nanowire layer （nearly 1 tim in thickness） and an underlying non- nanowire layer （at least 1 μm in thickness）. In both two cases, the as-formed nanowires are partly crystallized. Thermal stability investigation reveals that the net-like structure of the anodic nanowire film almost keeps unchanged at a temperature less than 400℃ but is totally destroyed when being calcinated at 600 ℃. In contrast, the nanowire layer formed by chemical method is stable even after being calcinated at 600 ℃. Our results also show that the uncalcinated or calcinated anodic films are much more photoactive than the corresponding films prepared by chemical oxidization. The difference in photoelectrochemical property of two types of films is discussed based on their microstructures.

关键词： Anodization Nanowires Thin films Titanium dioxide Titanate

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Highly performed platinum nanosheets synthesized under in situ reaction conditions for hydrogen generation

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Journal of Energy Chemistry 2020年第12期29卷 272-279页

作者： Xiaobing Bao Yutong Gong Xiaozhong Zheng Jiayi Chen Shanjun Mao Yong Wang Advanced materials and catalysis Group Institute of CatalysisZhejiang UniversityHangzhou 310028ZhejiangChina

Surface properties of a catalyst, especially exposed crystal facets and coordination states, directly affect the catalyst's performance. Herein, we illustrate how reaction conditions direct the fabrication of a wellbehaved catalyst with desired structures in the case of hydrogen evolution reaction(HER). Stable adsorbed PtClxions on CNTs are in situ electrochemically reduced into a unique Pt nanosheet structure enclosed by high-index(311) and low-index(200) and(111) facets during HER process. Experimental results and density functional theory(DFT) calculation disclose the function mechanism between these unique structures and reactants. The adsorbed H2 O and reactive species act as capping agents protecting the(311) facet where the dissociation of water molecule is promoted, and the produced H*intermediates favorably combine and release on the nearby low-index Pt sites. The joint collaborations of these active sites afford Pt nanosheets comparable activity to 20 wt% Pt/C and a 12.7-fold over mass activity. These findings provide novel insight into the synthesis of heterogeneous catalysts with high specificity.

关键词： Pt nanosheet Crystal growth Reaction condition Hydrogen evolution Heterogeneous catalysis

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