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Porous S-doped carbon nitride foam with accelerated charge dynamics for synchronous photocatalytic hydrogen production and highly selective oxidation of amines

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Nano Research 2024年第8期17卷 6860-6869页

作者： Yu He Aiping Wu Nan Wang Ying Xie Chungui Tian Honggang Fu key laboratory of Functional Inorganic Material chemistry(ministry of education of the People’s Republic of China) Heilongjiang UniversityHarbin 150080China

Photocatalytic hydrogen evolution coupled with organic oxidation holds great promise for converting solar energy into high-valueadded chemicals,but it is hampered by sluggish charge dynamics and limited redox ***,a porous S-doped carbon nitride(S-C_(3)N_(4−y))foam assembled from ultrathin nanosheets with rich nitrogen vacancies was synthesized using a molecular selfassembly *** S dopants and N vacancies synergistically adjusted the band structure,facilitating light absorption and enhancing the oxidation ***,the ultrathin nanosheets and porous structure provided more exposed active sites and facilitated mass and charge ***,S-C_(3)N_(4−y) foam exhibited enhanced photocatalytic activities for synchronous hydrogen evolution(4960μmol/(h·g))and benzylamine oxidation to N-benzylidenebenzylamine(4885μmol/(h·g))with high selectivity of>99%,which were approximately 17.6 and 72.9 times higher than those of bulk CN,*** photocatalytic coupling pairing reaction promotes the water splitting by consuming H2O2,thereby improving the hydrogen evolution efficiency and achieving the production of high value-added *** study provides an effective route for regulating the morphology and band structure of carbon nitride for synthesizing highly valuable chemicals.

关键词： photocatalysis S-doped carbon nitride band structure regulation hydrogen evolution coupled with benzylamine oxidation reaction mechanism

Recent progress of cobalt-based electrocatalysts for water splitting: Electron modulation, surface reconstitution, and applications

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Nano Research 2024年第4期17卷 2234-2269页

作者： Zhijian Liang Di Shen Lei Wang Honggang Fu key laboratory of Functional Inorganic Material chemistry Ministry of Education of the People’s Republic of ChinaHeilongjiang UniversityHarbin 150080China

Electrocatalytic water splitting is an essential and effective means to produce green hydrogen energy structures,so it is necessary to develop non-precious metal catalysts to replace precious ***-based catalysts present effective alternatives due to the diverse valence states,adjustable electronic structures,and plentiful *** this review,the catalytic mechanisms of hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)for electrocatalytic water splitting are ***,the synthesis strategies of various cobalt-based catalysts are systematically summarized,followed by the relationships between the structure and performance ***,the effects of d-band center and spin regulation for cobalt-based catalysts are also ***,the dynamic electronic and structural devolution of cobalt-based catalysts are elucidated by combining a series of in-situ ***,we highlight the challenges and future developed directions of cobalt-based catalysts for electrocatalytic water splitting.

关键词： cobalt-based electrocatalysts water splitting electron modulation surface reconfiguration

Progress and prospect of Pt-based catalysts for electrocatalytic hydrogen oxidation reactions

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Nano Research 2024年第3期17卷 960-981页

作者： Xu Zhang Ying Xie Lei Wang key laboratory of Functional Inorganic Material chemistry Ministry of Education of the People’s Republic of ChinaHeilongjiang UniversityHarbin 150080China

To achieve the goals of the peak carbon dioxide emissions and carbon neutral,the development and utilization of sustainable clean energy are extremely *** fuel cells are an important system for converting hydrogen energy into electrical ***,the slow hydrogen oxidation reaction(HOR)kinetics under alkaline conditions has limited its ***,elucidating the catalytic mechanism of HOR in acidic and alkaline media is of great significance for the construction of highly active and stable *** terms of practicality,Pt is still the primary choice for commercialization of fuel *** the above basis,we first introduced the hydrogen binding energy theory and bifunctional theory used to describe the HOR activity,as well as the pH *** that,the rational design strategies of Pt-based HOR catalysts were systematically classified and summarized from the perspective of activity *** addition,we further emphasized the importance of theoretical simulations and in situ characterization in revealing the HOR mechanism,which is crucial for the rational design of ***,the practical application of Pt-based HOR catalysts in fuel cells was also *** closing,the current challenges and future development directions of HOR catalysts were *** review will provide a deep understanding for exploring the mechanism of highly efficient HOR catalysts and the development of fuel cells.

关键词： Pt-based catalysts hydrogen oxidation reaction(HOR) electrocatalytic mechanism hydrogen binding energy theory bifunctional theory

Peroxisome Proliferator-Activated Receptor-γCoactivator-1αin the Spotlight with Multiple Sclerosis

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Neuroscience Bulletin 2024年第2期40卷 268-272页

作者： Ya-Na Yang Mao-Qing Zhang Feng-Lin Yu Bing Han Ming-Yue Bao Yan He Xing Li Yuan Zhang key laboratory of medicinal Resources and Natural Pharmaceutical chemistry(Shaanxi Normal University) The Ministry of EducationXi’an 710119China College of Life Sciences Shaanxi Normal UniversityXi’an 710119China

Multiple sclerosis(MS)is a chronic and incurable autoimmune disease of the central nervous system(CNS)that results in neuro-inflammation and *** therapies for MS alleviate symptoms to some extent but fail to realize myelin ***,it is crucial to identify effective targets to promote *** a widely expressed transcriptional regulator,peroxisome proliferatoractivated receptor-coactivator-1α(PGC-1α)expresses in different cells with high energy consumption,including skeletal muscle cells,brown fat cells,neurons,astrocytes,and oligodendrocyte precursor cell(OPC)[1].Targeting PGC-1αmay be beneficial for CNS development and various neurodegenerative diseases.

关键词： inflammation myelin autoimmune

Synergistic Ru/RuO_(2)heterojunctions stabilized by carbon coating as efficient and stable bifunctional electrocatalysts for acidic overall water splitting

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Nano Research 2024年第8期17卷 6931-6939页

作者： Man Wu Yuying Fan Yang Huang Dongxu Wang Ying Xie Aiping Wu Chungui Tian key laboratory of Functional Inorganic Material chemistry Ministry of Education of the People’s Republic of ChinaHeilongjiang UniversityHarbin 150080China

The development of highly active and stable acidic water oxidation electrocatalysts is of great significant for promoting the industrial application of proton exchange membrane ***-based catalysts have broad application prospects in acidic water oxidation,but their limitations in stability and activity hinder their further ***,a nitrogen-doped carbon(NC)coated porous Ru/RuO_(2)heterojunctional hollow sphere(Ru/RuO_(2)/NC)is designed as high-active and stable bifunctional electrocatalyst for acidic oxygen evolution reaction(OER)and hydrogen evolution reaction(HER).In synthesis,the key is to use mesoporous polydopamine spheres as a template for forming hollow spheres,a source of NC coating and a reducing agent for forming Ru/RuO_(2)*** Ru/RuO_(2)heterojunction adjusts the electronic structure of Ru active sites,optimizing the adsorption of intermediate ***,the NC coating and the interaction between NC and Ru/RuO_(2)effectively prevent Ru from over-oxidation and *** porous hollow structure provides more exposed active sites and promotes mass ***,Ru/RuO_(2)/NC exhibits outstanding OER and HER performance with low overpotentials of 211 and 32 mV at 10 mA·cm^(−2),respectively,and shows excellent *** acid water splitting electrolyzer,based on the bifunctional Ru/RuO_(2)/NC,requires low cell voltages of 1.46 and 1.76 V at 10 and 100 mA·cm^(−2),respectively,with good stability for over 100 h operation,surpassing Pt/C||RuO_(2)and most of the reported catalysts.

关键词： hollow heterojunction bifunctional electrocatalysts oxygen evolution hydrogen evolution acidic water splitting

Concerted Steric and Electronic Strategy in Thermostable Salicylaldiminato Nickel Catalysts for Ethylene(Co)polymerization

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Chinese Journal of Polymer Science 2024年第08期42卷 1085-1092页

作者： Hong-Yu Ji Hong-Liang Mu Chun-Feng Tang Yu-Xing Zhang Yue Chi Zhong-Bao Jian key laboratory of Advanced Structural Materials Ministry of Education School of Materials Science and Engineering Changchun University of Technology State key laboratory of Polymer Physics and chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences

Olefin polymerization is one of the most im portant chemical reactions in *** work presents a strategy that emphasizes the synergistic meta/poro-steric hindrance of N-aryl groups and electronic effects in newly synthesized neutral salicylaldiminato nickel *** nickel（Ⅱ） catalysts exhibit exceptional thermostability,ranging from 30℃ to 130℃,demonstrating enhanced catalytic activities and broadly regulated polyethylene molecular weights(3-341 kg·mol-1) and controlled polymer branch density（2-102 brs/1000C）.The preferred catalyst Ni3 with concerted steric and electronic effects enables the production of solid-state semi-crystalline polyethylene materials at temperatures below 90℃.Notably,Ni3 exhibits an impressive tolerance of 110℃ and can withstand even the challenging polymerization temperature of 130℃,leading to the production of polyethylene wax and ***,functionalized polyethylene is produced.

关键词： Nickel catalyst Oil Polyolefin Salicylaldiminato ligand Wax

Moisture‑Electric–Moisture‑Sensitive Heterostructure Triggered Proton Hopping for Quality‑Enhancing Moist‑Electric Generator

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Nano-Micro Letters 2024年第3期16卷 351-366页

作者： Ya’nan Yang Jiaqi Wang Zhe Wang Changxiang Shao Yuyang Han Ying Wang Xiaoting Liu Xiaotong Sun Liru Wang Yuanyuan Li Qiang Guo Wenpeng Wu Nan Chen Liangti Qu key laboratory of Cluster Science Ministry of Education of ChinaKey Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081People’s Republic of China Yangtze Delta Region Academy of Beijing Institute of Technology Jiaxing 314019People’s Republic of China Department of chemistry Key Laboratory of Organic Optoelectronics&Molecular EngineeringMinistry of EducationTsinghua UniversityBeijing 100084People’s Republic of China

Moisture-enabled electricity(ME)is a method of converting the potential energy of water in the external environment into electrical energy through the interaction of functional materials with water molecules and can be directly applied to energy harvesting and signal ***,ME can be unreliable in numerous applications due to its sluggish response to moisture,thus sacrificing the value of fast energy harvesting and highly accurate information ***,by constructing a moisture-electric-moisture-sensitive(ME-MS)heterostructure,we develop an efficient ME generator with ultra-fast electric response to moisture achieved by triggering Grotthuss protons hopping in the sensitized ZnO,which modulates the heterostructure built-in interfacial potential,enables quick response(0.435 s),an unprecedented ultra-fast response rate of 972.4 mV s^(−1),and a durable electrical signal output for 8 h without any *** research provides an efficient way to generate electricity and important insight for a deeper understanding of the mechanisms of moisture-generated carrier migration in ME generator,which has a more comprehensive working scene and can serve as a typical model for human health monitoring and smart medical electronics design.

关键词： Moist-electric generators Grotthuss proton hopping Fast response Durable electrical output Personal health monitoring

Nanocomposite: Keggin-type Co_(4)-polyoxometalate@cobaltporphyrin linked graphdiyne for hydrogen evolution in seawater

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Nano Research 2024年第3期17卷 1281-1287页

作者： Jiejie Ping Danyang He Fei Wang Nan Wang Yi-cheng Fu Zihao Xing Zhiyu Jia Guo-Yu Yang key laboratory of Cluster Science Ministry of EducationSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China key laboratory of Polyoxometalate and Reticular Material chemistry of ministry of education Facluty of Chmeistry Northeast Normal UniversityChangchun 130024China Peking University Third Hospital Beijing 100190China

Polyoxometalate-based nanocomposites with electrocatalytic activity have been applied in hydrogen evolution reactions(HER).Seawater as the main water resource on the earth should be developed as the water electrolysis to prepare high-purity *** this paper,we used two synthesis strategies to prepare the nanocomposite Co_(4)-POM@Co-PGDY(Co_(4)-POM:the Kegging-type microcrystals of K_(10)[Co_(4)(PW_(9)O_(3)4)2]and Co-PGDY:cobalt-porphyrin linked graphdiyne)with excellent activity for ***-PGDY as the porous material is applied not only as the protection of microcrystals towards the metal ion in seawater but also as the co-electrocatalyst of Co_(4)-***_(4)-POM@Co-PGDY exhibits excellent HER performance in seawater electrolytes with low overpotential and high stability at high ***,we have observed a key H_(3)O+intermediate emergence on the surface of nanocomposite during hydrogen evolution process in seawater by Raman synchrotron radiation-based Fourier transform infrared(SR-FTIR).The results in this paper provide an effective strategy for preparing polyoxometalate-based electrocatalysts with high-performance toward hydrogen evolution reaction.

关键词： polyoxometalate graphdiyne seawater hydrogen evolution reaction

A highly reduced Mo_(74) polyoxometalate featuring high proton conductivity accessed by building block strategy

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Science China chemistry 2024年第3期67卷 862-868页

作者： Shi-Yi Liu Xue-Xin Li Wei-Chao Chen Kui-Zhan Shao Xin-Long Wang Chao Qin Zhong-Min Su key laboratory of Polyoxometalate and Reticular Material chemistry of ministry of education Department of ChemistryNortheast Normal UniversityChangchun 130024China State key laboratory of Supramolecular Structure and Materials Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China

Highly reduced polyoxometalates(POMs) are predicted to be used as rather high energy density materials;however,it still suffers from the limited cluster species and reduction *** we demonstrate that it is possible to employ the building block strategy to generate a highly reduced polyoxomolybdate(C_(2)H_(8)N)_(14)(NH_(4))_(4)H_(14)[Mo_(48)-ⅤMo_(26)ⅥO_(202)(OH)_(12)(SO_(4))_(6)]·46H_(2)O(Mo_(74)).The fundamental Mo-based{Mo_x}(x=4,5,and 6) building blocks,which are templated by tetra-coordinated anions{MoO_(4)}or{SO_(4)},not only lay foundation for the formation of Mo_(74) featuring an unprecedented reduction ratio of 65%,but also give rise to SBBs-mediated(secondary building blocks) supramolecular dense packing interactions among the isolated Mo_(74) clusters that are favorable for proton ***,high proton conductivity(2.04×10^(-2)S cm^(-1)) had been realized at 50℃ and 90% relative humidity,revealing one of the well-known POMs-based crystalline proton conducting *** result highlights that this building block approach possesses great potential in producing highly reduced POM systems that can achieve controllable reduced ratio and desirable properties.

关键词： polyoxometalate building block molybdenum highly reduced state proton conduction