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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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Self-assembly of two pairs of homochiral M2L4 coordination capsules with varied confined space using Tr?ger's base ligands

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Chinese Chemical Letters 2025年第2期36卷 360-365页

作者： Yi Zhou Wei Zhang Rong Fu Jiaxin Dong Yuxuan Liu Zihang Song Han Han Kang Cai College of chemistry Nankai University department of chemistry Northwestern University department of chemistry The University of Hong Kong

Chiral coordination molecular cages/capsules with discrete nanoconfined chiral cavities demonstrate significant potential applications across various fields. In this study, we utilized Tr?ger's base as the building block to design and synthesize two pairs of enantiopure ligands. These ligands were then self-assembled with Pd(II) ions through chiral self-sorting coordination, resulting in the formation of two pairs of homochiral M2L4-type coordination molecular capsules. Notably, due to differences in the substitution positions on the Tr?ger's base, these two pairs of enantiomeric coordination molecular capsules exhibited distinct levels of cavity closures, cavity sizes, and host-guest recognition properties. This research offers valuable insights into the construction of novel chiral molecular capsules and the regulation of confined cavities.

关键词： Chirality Host-guest recognition Metal-organic capsule Self-sorting Tröger's base

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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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Enantioselective reductive conjugate alkenylation ofα,β-enones with keto alkenyl acetates by nickel catalysis

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Science China chemistry 2025年第1期68卷 157-162页

作者： Rong-De He Yun-Lei Luo Qiu-Quan Pan Qi-Wei Yao Xing-Zhong Shu State Key Laboratory of Applied Organic chemistry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China

Reactions involving alkenyl acetates offer cost-effective and environmentally friendly routes for alkene synthesis,yet their asymmetric variant remains ***,asymmetric conjugate alkenylation predominantly centered on nucleophilic addition using alkenyl–*** manuscript presents an asymmetric reductive conjugate alkenylation reaction involving alkenyl *** method facilitates the enantioselective addition of keto alkenyl groups toα,β-enones,resulting in the formation of unsaturated diketones—a class of useful structural motifs that are challenging to access *** use of electron-rich Pyroxy ligand is essential for achieving both high reaction efficiency and enantioselectivity.

关键词： nickel alkenylation asymmetric cross-coupling alkenes

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Critical new insights into the interactions of hexafluoropropylene oxide-dimer acid(GenX or HFPO-DA)with albumin at molecular and cellular levels

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Journal of Environmental Sciences 2025年第3期149卷 88-98页

作者： Shi-Ya Peng Ya-Di Yang Rong Tian Naihao Lu Jiangxi Key Laboratory of Green chemistry College of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang 330022China

A key characteristic to be elucidated,to address the harmful health risks of environmental perfluorinated alkyl substances(PFAS),is their binding modes to serum albumin,the most abundant protein in *** oxide-dimer acid(GenX or HFPO-DA)is a new industrial replacement for the widespread linear long-chain ***,the detailed interaction of new-generation short-chain PFAS with albumin is still ***,the binding characteristics of bovine serum albumin(BSA)to GenX were explored at the molecular and cellular *** found that this branched short-chain GenX could bind to BSA with affinity lower than that of legacy linear long-chain perfluorooctanoic acid(PFOA).Site marker competitive study and molecular docking simulation revealed that GenX interacted with subdomain IIIA to form BSA-GenX *** with its weaker affinity to albumin protein,the cytotoxicity of branched short-chain GenX was less susceptible to BSA binding compared with that of the linear long-chain *** contrast to the significant effects of strong BSA-PFOA interaction,the weak affinity of BSA-GenX binding did not influence the structure of protein and the cytotoxicity of *** detailed characterization and direct comparisons of serum albumin interaction with new generation short-chain GenX will provide a better understanding for the toxicological properties of this new alternative.

关键词： GenX Protein binding Albumin Cytotoxicity Risk assessment

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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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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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Synthesis of ternary geopolymers using prediction for effective solidification of mercury in tailings

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Journal of Environmental Sciences 2025年第1期147卷 392-403页

作者： Xuan Lu Jinfa Guo Fang Chen Mengkui Tian School of chemistry and Chemical engineering Guizhou UniversityGuiyang 550025China

This study used steel slag,fly ash,and metakaolin as raw materials(SFM materials)to create silica-alumina-based geopolymers that can solidify Hg^(2+)when activated with sodiumbased water *** experiments began with a triangular lattice point mixing design experiment,and the results were fitted,analyzed,and *** optimum SFM material mass ratio was found to be 70%steel slag,25%fly ash,and 5%*** optimum modulus of the activator was identified by comparing the unconfined compressive strength and solidifying impact on Hg^(2+)of geosynthetics with different *** SFM geopolymer was then applied in the form of potting to cure the granulated mercury *** inclusion of 50%SFM material generated a geosynthetic that reduced mercury transport to the surface soil by roughly 90%.The mercury concentration of herbaceous plant samples was also reduced by 78%.It indicates that the SFM material can effectively attenuate the migration transformation of ***,characterization methods such as XPS and FTIR were used to investigate the mechanism of Hg^(2+)solidification by geopolymers generated by SFM *** possible solidification mechanisms were proposed as alkaline environment-induced mercury precipitation,chemical bonding s,surface adsorption of Hg^(2+)and its precipitates by the geopolymer,and physical encapsulation.

关键词： Mercury Geopolymer Solidification Tailings

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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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