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Atomically precise M-N-C electrocatalysts for oxygen reduction:Effects of inter-site distance,metal-metal interaction,coordination environment,and spin states

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Journal of Energy chemistry 2025年第2期101卷 132-155页

作者： Junfeng Huang Saira Ajmal Anuj Kumar Jianwen Guo Mohammed Mujahid Alam Abdullah G.Al-Sehemi Ghulam Yasin School of Mechanical engineering Dongguan University of Technology Nano-Technology Research Laboratory Department of Chemistry GLA University department of chemistry College of Science King Khalid University School of Environmental Science and engineering Tianjin University State Key Laboratory of Chemical Resource engineering College of Materials Science and Engineering Beijing University of Chemical Technology

Inspired by molecular catalysts,researchers developed atomically precise nitrogen-coordinated single or dual metal sites imbedded in graphitized carbon（M-N-C） to fully utilize metallic sites for *** catalysts performed remarkably well in the electrocatalytic oxygen reduction reaction（ORR） due to their distinct coordination and electrical structures,Nonetheless,their maximum efficacy in practical applications has yet to be *** agenda identifies tailoring the coordination environment,spin states,intersite distance,and metal-metal interaction as innovative approaches to regulate the ORR performance of these ***,it is necessary to undertake a precise assessment of these methodologies and the knowledge obtained to be implemented in the design of future M-N-C catalysts for ***,this review aims to analyze recent progress in M-N-C ORR catalysts,emphasizing their innovative engineering with aspects such as alteration in intersite distance,metal-metal interaction,coordination environment,and spin ***,we critically discuss how to logically monitor the atomic structure,local coordination,spin,and electronic states of M-N-C catalysts to modulate their ORR *** have also highlighted the challenges associated with M-N-C catalysts and proposed suggestions for their future design and fabrication.

关键词： Activity descriptors Electrocatalysis M-N-C electrocatalysts ORR Spin states

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Electrocatalytic selective synthesis and tandem utilization of hydroxylamine

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Science China chemistry 2025年

作者： Yuxuan Lu Hengquan Yang engineering Research Center of Ministry of Education for Fine Chemicals School of Chemistry and Chemical Engineering Shanxi Key Laboratory of Green Catalytic Synthesis of Coal-based High Value Chemicals Shanxi University

The transformation of renewable nitrogen feedstock to nitrogenous chemicals plays a significant role in our modern society,considering the crucial impact of nitrogenous chemicals on life sciences,biomedicine,agriculture,and *** （NH2OH）,a typical nucleophile,has been widely served as the nitrogenous feedstock to produce nitrogenous *** NH2OH synthesis methods rely on harsh reaction conditions,leading to an unfavorable environmental *** contrast,nitric oxide electroreduction promises to produce NH2OH powered by renewable *** achievements have revealed the possibility of this process,but have also identified significant *** activity and selectivity are fundamentally limited by competing hydrogenation reactions,while the performance evaluation with high accuracy and reproducibility is ***,this review aims to provide insight into the mechanism of NH2OH electrosynthesis,especially regarding understanding reaction pathways and the design principle towards efficient ***,the performance evaluation parameters and standard measurement methods for NH2OH synthesis are summarized to screen efficient ***,the prospects and emerging opportunities to synthesize nitrogen-containing organic compounds by tandem reaction are *** review aims to provide a guide for evaluating and exploring efficient electrocatalytic systems for NH2OH production and utilization technology.

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Enantioselective copper-catalyzed dearomative borylative cyclization of indoles and mechanistic insights

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Science China chemistry 2025年第2期68卷 670-678页

作者： Yanfei Li Xuetao Li Zheng Zhang Yiliang Zhang Xiuping Yuan Jianjun Yin Simin Wang Wei Guan Qian Zhang Tao Xiong Jilin Province Key Laboratory of Organic Functional Molecular Design&Synthesis Department of ChemistryNortheast Normal UniversityChangchun 130024China Institute of Functional Material chemistry Department of ChemistryNortheast Normal UniversityChangchun 130024China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of chemistry and Chemical engineering Harbin Normal UniversityHarbin 150025China

Alicyclic nitrogen heterocycles,such as enantioenriched polycyclic fused[1,2-a]indoline derivatives,are widespread in natural products,agrochemicals and pharmaceutical *** methods predominantly rely on the recent emerging Heck-type catalytic asymmetric dearomatization(CADA)protocol,wherein noble palladium catalysts commonly necessitate the form arylPd species-triggered these *** contrast,a more sustainable base metal catalysis paradigm through alkyl metal species disrupting the aromaticity,that is,the utilization of challenging asymmetric Csp3–Csp3 bond formation entry to such important chiral densely functionalized polycyclic molecular scaffolds,remains an elusive ***,we report the first copper-catalyzed dearomative borylative cyclization of indoles under mild reaction conditions,affording an array of valuable Bpin-containing pyrrolo-fused[1,2-a]indolines bearing four consecutive stereogenic centers with excellent enantioand *** synthetic potential was documented via an array of useful *** functional theory(DFT)calculation studies elucidated the origin of the chemo-,regio-,enantio-and diastereoselectivities of this conversion.

关键词： copper catalysis dearomatization borylative cyclization indoles DFT calculations

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The controlled oxidation states of the H4PMo11VO40 catalyst induced by plasma for the selective oxidation of methacrolein

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Chinese Chemical Letters 2025年第2期36卷 189-194页

作者： Gang Hu Chun Wang Qinqin Wang Mingyuan Zhu Lihua Kang School of chemistry and Chemical engineering/State Key Laboratory Incubation Base for Green Processing of Chemical engineering Shihezi University College of chemistry&Chemical engineering Yantai University

In this paper,low-temperature dielectric-blocked discharge plasma （DBD） was employed for the first time to treat silica-doped H4PMo11VO40（HPAV） catalysts (DBD（Ar/x）-MF-Catal) and apply them in the catalytic methacrolein （MAL） selective oxidation to produce methacrylic acid （MAA）.This work investigates in detail the controllable regulation of the concentration of oxidation states on silica-doped HPAV catalysts by adjusting the DBD discharge with controlled changes in voltage,current,treatment time,and treatment *** reports the intrinsic correlation between oxidation states and MAL oxidation *** research results indicated that the catalytic performance was related to the presence of oxygen vacancies and oxygen species (VO2+),and are the main reason for the selective oxidation of MAL to ***,the generation of oxygen vacancies and VO2+altered localized electrons,which resulted in the easier activation of *** calculations of DFT also proved the formation mechanism of oxygen vacancies and VO2+and electron properties on high-performance polymers,which elucidated the intrinsic influence of catalyst *** DBD（Ar/10）-MF-Catal catalysts with suitable VO2+and oxygen vacancy concentrations exhibited the highest catalytic performance with 90%MAL conversion and 70%MAA selectivity and showed good stability （500 h）.

关键词： Catalyst Dopant Methacrolein Methacrylic acid Oxygen vacancy Plasma

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Constructing diverse switchable circularly polarized luminescence via a single azobenzene polymer film

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Chinese Chemical Letters 2025年第1期36卷 299-305页

作者： Xiang Wang Qingping Song Zixiang He Gong Zhang Tengfei Miao Xiaoxiao Cheng Wei Zhang State and Local Joint engineering Laboratory for Novel Functional Polymeric Materials Department of Polymer Science and EngineeringCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China School of Chemical and Environmental engineering Anhui Polytechnic UniversityWuhu 241000China Jiangsu Key Laboratory for chemistry of Low-Dimensional Materials School of Chemistry and Chemical EngineeringHuaiyin Normal UniversityHuaian 223300China

Recently circularly polarized luminescence(CPL)materials have attracted significant *** reversible dynamic property to these materials has been a key focus in cutting-edge fields,such as in high-level information ***,we provided a novel and general strategy involving handednessselective filtration and ground-state chiral self-recovery(CSR)in double film system to address this *** on this strategy,we achieved CPL switch through the reversible modulation of ground-state chirality including absorption and scattering circular dichroism(CD)signals over the full UV-visible wavelength range(365-700 nm)in a single azobenzene polymer(PAzo)*** importantly,by flexibly changing the type of fluorescent films,it is convenient to achieve general excited-state CSR,that is reversible switching of full-color including ideal white(CIE coordinate(0.33,0.33)),as well as room-temperature phosphorescent *** these CPL signals without almost any intensity decay after three cycles of onand-off *** results indicated that the trans-cis isomerization and ordered rearrangement of azobenzene units in PAzo film were the fundamental reasons for realizing CPL ***,based on this system we achieved dynamic visual encryption and decryption process including multiple decryption *** study provides an effective method for constructing a universally applicable chiroptical switch in excited state.

关键词： Circularly polarized luminescence Azobenzene polymer Multiple CPL Chiral switch Information encryption

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Synthesis of ordered mesoporous crystalline boron phosphate scaffold with double diamond surface structure

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Science China chemistry 2025年第2期68卷 590-600页

作者： Chao Wang Wen-Duo Lu Jiao Wang Shunai Che An-Hui Lu Lu Han School of Chemical Science and engineering Tongji UniversityShanghai 200092China State Key Laboratory of Fine Chemicals Liaoning Key Laboratory for Catalytic Conversion of Carbon ResourcesSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China School of chemistry and Chemical engineering Frontiers Science Center for Transformative MoleculesState Key Laboratory of Metal Matrix CompositesShanghai Key Laboratory for Molecular Engineering of Chiral DrugsShanghai Jiao Tong UniversityShanghai 200240China

Ordered mesoporous materials have received great attention due to their well-defined pore structures and potential applications in catalysis,adsorption,separation,drug delivery,*** various compositions of mesoporous solids have been successfully prepared,the preparation of crystalline non-metallic oxyacid salts with ordered mesoporosity remains a major ***,we report the synthesis of a mesoporous solid acid crystalline boron phosphate(BPO_(4))catalyst with a bicontinuous shifted double diamond(SDD)hyperbolic surface *** BPO_(4) scaffold was obtained by synergistic selfassembly in a mixed solvent of water and tetrahydrofuran using the diblock copolymer poly(ethylene oxide)-block-polystyrene as template and phosphoric acid and orthoboric acid as inorganic *** structure consists of two sets of diamond networks adjacent to each other with a mesostructural scale tetragonal symmetry(space group I4_(1)/amd)with unit cell parameters of a=80 nm and c=113 nm,which affords the scaffold a specific surface area of 44 m^(2)/*** a solid acid catalytic material,the SDD BPO_(4) scaffold exhibited excellent catalytic activity at room temperature with a conversion of furfural to 2-(dimethoxymethyl)furan over 70%and can be reused after recovery without serious loss of *** the propane oxidative dehydrogenation reaction,SDD BPO_(4) demonstrated high olefin productivity and selectivity while maintaining high reaction *** study provides ideas for the preparation of ordered mesoporous crystalline catalytic materials and demonstrates their potential for practical applications.

关键词： boron phosphate mesoporous material self-assembly block copolymer catalyst

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Unilamellar MnO_(2)nanosheets confined Ru-clusters combined with pulse electrocatalysis for biomass electrooxidation in neutral electrolytes

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Science Bulletin 2025年第2期70卷 193-202页

作者： Yuanqing He Chongyang Ma Shiheng Mo Chung-Li Dong Wei Chen Shuo Chen Huan Pang Renzhi Ma Shuangyin Wang Yuqin Zou School of chemistry and Chemical engineering Yangzhou UniversityYangzhou 225009China State Key Laboratory of Chem/Bio-Sensing and Chemometrics Advanced Catalytic Engineering Research Center of the Ministry of EducationCollege of Chemistry and Chemical EngineeringThe National Supercomputer Centers in ChangshaHunan UniversityChangsha 410082China department of Physics Tamkang UniversityNew Taipei City 25137China School of Materials Science and engineering Central South UniversityChangsha 410083China International Research Center for Materials Nanoarchitectonics(WPI-MANA) National Institute for Materials Science(NIMS)TsukubaIbaraki 305-0044Japan

The electrochemical oxidation of 5-hydroxymethylfurfural(HMFOR)in alkaline electrolyte is a promising strategy for producing high-value chemicals from biomass ***,the disproportionation of aldehyde groups under strong alkaline conditions and the polymerization of HMF to form humic substances can impact the purity of 2,5-furandicarboxylic acid(FDCA)*** use of neutral electrolytes offers an alternative environment for electrolysis,but the lack of OH^(-)ions in the electrolyte often leads to low current density and low yields of *** this study,a sandwich-structured catalyst,consisting of Ru clusters confined between unilamellar MnO_(2)nanosheets(S-Ru/MnO_(2)),was used in conjunction with an electrochemical pulse method to realize the electrochemical conversion of5-hydroxymethylfurfural into FDCA in neutral *** electrolysis and the strong electron transfer between Ru clusters and MnO_(2)nanosheets help maintain Ru in a low oxidation state,ensuring high *** increased*OH generation led to a groundbreaking current density of 47 mA/cm^(2)at1.55 V *** hydrogen electrode(RHE)and an outstanding yield rate of 98.7%for FDCA in a neutral *** work provides a strategy that combines electrocatalyst design with an electrolysis technique to achieve remarkable performance in neutral HMFOR.?2024 Science China *** by Elsevier *** Science China *** rights are reserved,including those for text and data mining,AI training,and similar technologies.

关键词： Electrocatalytic 5-hydroxymethylfurfural oxidation Neutral electrolyte Electrocatalysts Nano-confined structure Electrochemical pulse

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Construction of N-doped copper metal-organic frameworks for promoting photocatalytic carbon dioxide reduction to ethylene

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Science China chemistry 2025年第2期68卷 601-609页

作者： Fan Guo Zong-Zheng He Peng Wang Xiao-Yu Zhang Hongjian Yu Qin-Chao Wang Wei-Yin Sun School of chemistry and Chemical engineering Yangzhou UniversityYangzhou 225002China Coordination chemistry Institute State Key Laboratory of Coordination ChemistrySchool of Chemistry and Chemical EngineeringNanjing National Laboratory of MicrostructuresCollaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210023China

engineering nonmetallic atom-doped metal-organic framework(MOF)catalyst to promote C−C coupling and realize conversion of CO_(2) into C_(2 )multi-carbon hydrocarbon products is still ***,with 2-methylimidazole as a dopant of N element,an N-doped NH_(2)-CuBDC catalyst was obtained via a facile and simple stirring *** illumination,compared with catalytic CO_(2) reduction to C1 product of CO by original MOF,N-doped NH_(2)-CuBDC can motivate generation of C_(2)H_(4),which is difficult to achieve in photocatalytic system by MOF-based *** transfer rates of photo-generated charges have been expedited due to the high electron density around Cu catalytic sites after *** importantly,C–C coupling intermediate CO–CHO*was identified by in situ Fourier transform infrared spectroscopy during the catalytic CO_(2) reduction reaction process,which further indicates the presence of Cu–N sites in the NH_(2)-CuBDC can facilitate the formation of C2H_(4) *** work uncovers a new paradigm to design photocatalysts for enhancing the reduction of CO_(2) to C_(2) products.

关键词： metal-organic frameworks C-C coupling doping photocatalytic CO_(2) reduction Cu-based catalysts

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Novel photoresponsive dinuclear nickel catalysts for ethylene (co)polymerization

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Science China chemistry 2025年第2期68卷 714-722页

作者： Chenlong Nan Tong Pang Jiaxing Zhao Lijia Fan Chen Zou Xin-Qi Hao Mao-Ping Song Jun-Fang Gong Changle Chen Hui Jiang College of chemistry Pingyuan LaboratoryZhengzhou UniversityZhengzhou 450001China CAS Key Laboratory of Soft Matter chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China

Compared with the conventional strategies of electronic and/or steric perturbation,catalytic olefin polymerization modulated by light irradiation or metal-metal cooperativity effect is a fascinating challenge that attracts considerable attention in the academic *** this context,we design a strategy that could employ both effects to influence the polymerization *** dinuclear salicylaldimine andα-imino-ketone nickel complexes bearing a stiff-stilbene bridge were prepared,which could transfer between(E)-isomers and(Z)-isomers under ultraviolet *** isomerization can tune the electronic,steric and metal-metal cooperativity effects of the nickel *** this way,the catalytic activity,as well as polymer microstructures including molecular weight and branching density can be modulated in ethylene polymerization and copolymerization *** strategy is generally applicable to other olefin polymerization catalytic systems and other types of transition metal mediated catalysis.

关键词： photoresponsive dinuclear catalyst nickel(II) polar monomer olefin copolymerization

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CO_(2)-mediated bicarbonate conversion to concentrated formate in a CEM-based electrolyzer

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Journal of Energy chemistry 2025年第1期100卷 605-611页

作者： Haocheng Xiong Donghuan Wu Haonan Li Andrew Li Qikun Hu Siyao Song Bingjun Xu Qi Lu State Key Laboratory of Chemical engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China College of chemistry and Molecular engineering Peking UniversityBeijing 100871China Ordos Laboratory Inner Mongolia 017000China

Renewable energy-driven bicarbonate conversion to valuable chemicals presents an attractive strategy for mitigating CO_(2)emissions,as bicarbonate can be efficiently generated from the capture of atmospheric CO_(2)using alkaline solutions with reactive *** this work,we present a CO_(2)-mediated bicarbonate conversion to pure formate using a cation exchange membrane-based electrolyzer with a 25 cm^(2)electrode *** electrolysis achieved selectivities exceeding 75%for formate at a total current of 2.5 A,achieving formate concentrations up to 1.2 M and yields as high as 95%over extended *** techno-economic assessment confirmed the economic viability of the process,highlighting the potential for bicarbonate electrolysis as a sustainable method for producing valuable chemicals.

关键词： Electrocatalysis Techno-economic assessments Electrochemistry Flow electrolyzer

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