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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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Universal design of three-dimensional porous graphene-iron based promotors for kinetically rationalized lithium-sulfur chemistry

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Journal of Energy Chemistry 2025年第1期100卷 192-200页

作者： Hua Gao Yunfeng Zhang Menglei Wang Ruoxuan Yang Shuai Feng Xuan Cao Yaping Zhang Zhongyuan Lu Yingze Song State Key laboratory of environment-Friendly Energy materials School of Materials and Chemistry Southwest University of Science and Technology School of Material Science and Engineering Henan University of Technology College of Chemistry and Chemical Engineering Taishan University

Lithium-sulfur （Li-S） batteries are widely deemed to be one of the most potential candidates for future secondary batteries because of their remarkable energy ***,notorious polysulfide shuttling and retarded sulfur reaction kinetics pose significant obstacles to the further application of Li-S *** rationally designed highly active electrocatalysts can facilitate polysulfide conversion,the universal and scalable synthesis strategies need to be ***,a universal synthetic strategy to construct a series of three-dimensional （3D） porous graphene-iron （3DGr-Fe） based electrocatalysts involving 3DGr-FeP,3DGr-Fe3C,and 3DGr-Fe3Se4is exploited for manipulating the Li-S redox *** has been observed that the implementation of a 3D porous Gr architecture leads to the well-designed conductive networks,while the uniformly dispersed iron nanoparticles introduce an abundance of active sites,fostering the lithium polysulfide conversion,thereby bolstering the overall electrochemical *** Li-S battery with the 3DGr-Fe based electrocatalyst exhibits remarkable capacity retention of 94.8%upon 100 times at 0.2 ***,the soft-packaged Li-S pouch cell based on such a 3DGr-Fe electrocatalyst delivers superior capacity of 1060.71 mA h g-1and guarantees for the continuous 30 min work of fan *** investigation gives comprehensive insights into the design,synthesis,and mechanism of 3DGr-Fe based electrocatalysts with high activity toward efficient and durable Li-S batteries.

关键词： Lithium-sulfur battery Universal synthesis 3D graphene-iron based promotor 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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Controllable synthesis of biomimetic wood stem nanoporous high entropy oxides catalysts for oxygen evolution reaction

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Nano Research 2025年第1期18卷 107-117页

作者： Wei Wang Weiqi Wang Huihui Wang Xing Lu Jinwen Zhang Yunzhuo Lu School of materials Science and Engineering Dalian Jiaotong UniversityDalian 116028China School of Intelligence and Electronic Engineering Dalian Neusoft University of InformationDalian 116023China Guangdong Key laboratory of materials and Equipment in Harsh Marine environment Guangzhou Maritime UniversityGuangzhou 510725China

Bubbles generated during the oxygen evolution reaction(OER)in water splitting readily adhere to the electrode surface,thereby impeding contact between the electrolyte and the active sites,thereby increasing the ***,it is imperative to elucidate the bubble release behavior and engineer electrodes that facilitate faster bubble *** this study,inspired by the wood stem of the Norway spruce,we synthesized a gradient nanoporous high-entropy oxide(GNP-HEO)electrode with a controllable pore *** GNP-HEO,featuring a well-controlled gradient in pore size,is achieved through a straightforward strategy combining selective laser melting with selective phase *** unique gradient nanoporous structure not only facilitates bubble release but also diminishes the bubble shielding effect in OER,thereby enhancing electrocatalytic *** affect interaction of Al,Co,Cr,Fe,and Ni,coupled with the gradient nanoporous structure,yields exceptional OER performance,evidenced by an overpotential of 250 mV at a current density of 50 mA/cm^(2) and a Tafel slope of 38.0 mV/dec in 1 M *** functional theory calculations confirm that the GNPHEO adheres to the adsorbate evolution mechanism reaction pathway and exhibits significant *** work highlights a promising approach for the design and synthesis of high-performance OER electrocatalysts.

关键词： oxygen evolution reaction high-entropy oxides selective phase dis-solution selective laser melting gradient nanoporous

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Multiple Tin Compounds Modified Carbon Fibers to Construct Heterogeneous Interfaces for Corrosion Prevention and Electromagnetic Wave Absorption

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Nano-Micro Letters 2025年第1期17卷 507-527页

作者： Zhiqiang Guo Di Lan Zirui Jia Zhenguo Gao Xuetao Shi Mukun He Hua Guo Guanglei Wu Pengfei Yin College of Science Sichuan Agricultural UniversityYa’an 625014People’s Republic of China School of materials Science and Engineering Hubei University of Automotive TechnologyShiyan 442002People’s Republic of China Institute of materials for Energy and environment State Key Laboratory of Bio‑Fibers and Eco‑TextilesCollege of Materials Science and EngineeringQingdao UniversityQingdao 266071People’s Republic of China Shaanxi Key laboratory of Macromolecular Science and Technology School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’anShaanxi 710072People’s Republic of China

Currently,the demand for electromagnetic wave(EMW)absorbing materials with specific functions and capable of withstanding harsh environments is becoming increasingly ***-component interface engineering is considered an effective means to achieve high-efficiency EMW ***,interface modulation engineering has not been fully discussed and has great potential in the field of EMW *** this study,multi-component tin compound fiber composites based on carbon fiber(CF)substrate were prepared by electrospinning,hydrothermal synthesis,and high-temperature thermal *** utilizing the different properties of different substances,rich heterogeneous interfaces are *** effectively promotes charge transfer and enhances interfacial polarization and conduction *** prepared SnS/SnS_(2)/SnO_(2)/CF composites with abundant heterogeneous interfaces have and exhibit excellent EMW absorption properties at a loading of 50 wt%in epoxy *** minimum reflection loss(RL)is−46.74 dB and the maximum effective absorption bandwidth is 5.28 ***,SnS/SnS_(2)/SnO_(2)/CF epoxy composite coatings exhibited long-term corrosion resistance on Q235 steel ***,this study provides an effective strategy for the design of high-efficiency EMW absorbing materials in complex and harsh environments.

关键词： Electrostatic spinning Component regulation Heterogeneous interfaces Electromagnetic wave absorption Corrosion protection

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Depression mechanism of sulfite ions on sphalerite and Pb^(2+)activated sphalerite in the flotation separation of galena from sphalerite

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International Journal of Minerals,Metallurgy and materials 2025年第2期32卷 335-345页

作者： Feng Zhang Chenyang Zhang Linlin Wu Wei Sun Hongliang Zhang Jianhua Chen Yong Pei Songjiang Li Engineering Research Center of Ministry of Education for Carbon Emission Reduction in Metal Resource Exploitation and Utilization Hunan International Joint Research Center for Efficient and Clean Utilization of Critical Metal Mineral ResourcesSchool of Minerals Processing and BioengineeringCentral South UniversityChangsha 410083China State Key laboratory of Mineral Processing Beijing General Research Institute of Mining&MetallurgyBeijing 100160China Hunan Provincial Key laboratory of Micro&Nano materials Interfaces Science College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China School of Resources Environment and MaterialsGuangxi UniversityNanning 530004China Department of Chemistry Xiangtan UniversityXiangtan 411105China China Railway Resource Group Co.Ltd Beijing 102300China

The depression mechanism of sulfite ions on sphalerite and Pb^(2+)activated sphalerite in the flotation separation of galena from sphalerite still lacked in-depth ***,the depression mechanism of sulfite ions on sphalerite and Pb^(2+)activated sphalerite in the flotation separation of galena from sphalerite was further systematically investigated with experiments and density functional theory(DFT)*** X-ray photoelectric spectroscopy(XPS)results,DFT calculation results,and frontier molecular orbital analysis indicated that sulfite ions were difficult to be adsorbed on sphalerite surface,suggesting that sulfite ions achieved depression effects on sphalerite through other non-adsorption ***,the oxygen content in the surface of sphalerite treated with sulfite ions in creased,which enhanced the hydrophilicity of the sphalerite and further increased the difference in hydrophilicity between sphalerite and ***,sulfite ions were chelated with lead ions to form PbSO_(3)in *** hydrophilic PbSO_(3)was more easily adsorbed on sphalerite than *** interaction between sulfite ions and lead ions could effectively inhibit the activation of *** addition the UV spectrum showed that after adding sulfite ions,the peak of perxanthate in the sphalerite treated xanthate solution was significantly stronger than that in the galena with xanthate solution,indicating that xanthate interacted more readily with sulfite ions and oxygen mo lecules within the sphalerite system,leading to the formation of ***,sulfite ions hardly depressed the flotation of ga lena and could promote the flotation of galena to some *** study deepened the understanding of the depression mechanism o sulfite ions on sphalerite and Pb^(2+)activated sphalerite.

关键词： sphalerite galena sulfite ion density functional theory depression mechanism

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Prussian Blue Analogue‑Templated Nanocomposites for Alkali‑Ion Batteries:Progress and Perspective

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Nano-Micro Letters 2025年第1期17卷 216-261页

作者： Jian‑En Zhou Yilin Li Xiaoming Lin Jiaye Ye Key laboratory of Theoretical Chemistry of environment Ministry of EducationSchool of ChemistrySouth China Normal UniversityGuangzhou 510006People’s Republic of China School of Chemistry and Physics Faculty of ScienceQueensland University of Technology2 George StreetBrisbaneQLD 4000Australia Centre for materials Science Queensland University of Technology2 George StreetBrisbaneQLD 4000Australia

Lithium-ion batteries(LIBs)have dominated the portable electronic and electrochemical energy markets since their commercialisation,whose high cost and lithium scarcity have prompted the development of other alkali-ion batteries(AIBs)including sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs).Owing to larger ion sizes of Na^(+)and K^(+)compared with Li^(+),nanocomposites with excellent crystallinity orientation and well-developed porosity show unprecedented potential for advanced lithium/sodium/potassium *** enticing open rigid framework structures,Prussian blue analogues(PBAs)remain promising self-sacrificial templates for the preparation of various nanocomposites,whose appeal originates from the well-retained porous structures and exceptional electrochemical activities after thermal *** review focuses on the recent progress of PBA-derived nanocomposites from their fabrication,lithium/sodium/potassium storage mechanism,and applications in AIBs(LIBs,SIBs,and PIBs).To distinguish various PBA derivatives,the working mechanism and applications of PBA-templated metal oxides,metal chalcogenides,metal phosphides,and other nanocomposites are systematically evaluated,facilitating the establishment of a structure–activity correlation for these *** on the fruitful achievements of PBA-derived nanocomposites,perspectives for their future development are envisioned,aiming to narrow down the gap between laboratory study and industrial reality.

关键词： Prussian blue analogues Self-sacrificial template Lithium-ion batteries Sodium-ion batteries Potassium-ion batteries

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A2B2O7 pyrochlore compounds:A category of potential materials for clean energy and environment protection catalysis

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Journal of Rare Earths 2020年第8期38卷 840-849,I0001页

作者： Junwei Xu Rong Xi Xianglan Xu Yan Zhang Xiaohui Feng Xiuzhong Fang Xiang Wang Key laboratory of Jiangxi Province for environment and Energy Catalysis College of ChemistryNanchang UniversityNanchang 330031China

A2B2O7 pyrochlore is a kind of important functional materials for different purposes,which has been investigated extensively by crystallographers and material ***,the catalytic chemistry of this type of special compounds has rarely been documented,though a few researchers have tried to synthesize some pyrochlore compounds with different chemical compositions for a variety of green energy production and air pollution control reactions in the *** the expectation to help catalysis scientists to get better acquaintance with,and gain deeper understanding on this type of compounds as heterogeneous catalysts,the major publications over the past several decades have been screened and reviewed in this paper,based also on our own experience of studying on this type of catalytic *** crystalline phase transformations of the compounds with the change of the A and B site cations,the phase change’s influences on the surface and bulk properties,and their subsequent impact on the catalytic performance for different reactions have been ***,the future work which needs to be performed to perceive in depth this kind of important materials as catalysts has been proposed and *** trust that this short review contains valuable information,which will provide great help for people to get better cognition for A2 B2 O7 pyrochlore compounds,and assist them to develop better catalysts for various reactions.

关键词： A2B2O7 pyrochlore compounds Crystalline phase change Lattice and surface oxygen vacancies Value-added CH4 transformation Air pollution control reactions Rare earths

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2D phosphides heterostructures on titanium microfiltration membrane for enhanced ampere-level current density overall seawater splitting

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Nano Research 2025年第1期18卷 249-259页

作者： Wenjing Dai Xin Wang Yulong Ma Sisi He Ming Chen Zhaohui Yin Shuheng Tian Maolin Wang Shixiang Yu Hang Zhang Yuanzhe Wang Hong Wang Jianxin Li Faming Gao Bowen Cheng Yun Wang Zhen Yin Ding Ma Tianjin Key laboratory of Brine Chemical Engineering and Resource Eco-utilization College of Chemical Engineering and Materials ScienceTianjin University of Science and TechnologyTianjin 300457China State Key laboratory of Biobased Fiber Manufacturing Technology Tianjin University of Science and TechnologyTianjin 300457China Haian Institute of High-Tech Research Nanjing UniversityHaian 226600China Beijing National laboratory for Molecular Sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China State Key laboratory of Separation Membranes and Membrane Processes Separation Membrane Science and Technology International Joint Research CentreTiangong UniversityTianjin 300387China Centre for Catalysis and Clean Energy School of Environment and ScienceGold Coast CampusGriffith UniversitySouthportQueensland 4222Australia

The advancement of direct seawater electrolysis is a significant step towards sustainable hydrogen production,addressing the critical need for renewable energy sources and efficient resource ***,direct seawater electrolysis has to face several challenges posed by the corrosiveness of highly concentrated chloride and the competitive chlorine evolution reaction(ClER).To overcome these issues,we designed a novel NiP_(2)@CoP electrocatalyst on a porous titanium microfiltration(Ti MF)*** obtained bifunctional NiP_(2)@CoP catalyst outperforms the Pt/C and IrO_(2),as evidenced by its low overpotentials of 192 and 425 mV at a current density of 500 mA·cm^(-2) for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)in alkaline seawater(1 M KOH+0.5 M NaCl),***,only 231 and 569 mV overpotentials are required at the current density of 1500 mA·cm^(-2) towards HER and OER in alkaline seawater,*** importantly,no ClER was observed,demonstrating its excellent selectivity to *** selection of porous Ti MF membrane as an electrode substrate further enhances the performance by providing a robust structure that promotes the fast generation and release of gas *** promising outcomes obtained with NiP_(2)@CoP catalysts on Ti MF support,therefore,pave the way for the commercial viability of direct seawater electrolysis technologies at industrial-level current densities.

关键词： direct seawater electrolysis porous titanium microfiltration membrane phosphides heterostructures NiP_(2)@CoP electrocatalyst excellent selectivity to oxygen evolution reaction(OER)

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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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