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Potassium ions and cyano group modified g-C3N4 for effective generation of H2O2 through two-electron oxygen reduction

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Science China chemistry 2025年第1期68卷 192-200页

作者： Dongying Wang Shulan Pu Yongmin Chen Ke Lei Yujie Duan Linjiao Mao Xuhui Zeng Xi Luo Yuntao Zhang Yuqin Dong Jin Zhong Zhang Yan Sun School of Mechanical Engineering Chengdu University Department of chemistry and Biochemistry University of California

Potassium ions （K+） doped graphitic carbon nitride （g-C3N4） was prepared by a thermal etching method using potassium hydroxide （KOH） as an ion *** transform infrared spectroscopy （FTIR） and X-ray photoelectron spectroscopy （XPS）results showed that the generation of the cyano group was detected while introducing K+.Under simulated sunlight irradiation,the sample with a K+doping amount of 10%showed the highest hydrogen peroxide （H2O2） generation rate of2,140.2μmol *** apparent quantum yield （AQY） at 400 nm and the solar-to-chemical conversion （SCC） are 4.35%and1.23%,respectively.K+acted as a bridge between g-C3N4layers,which enhanced charge transfer ***,the cyano group enhanced the adsorption capacity of protons （H+） and promoted the yield of *** catalyst exhibited excellent photocatalytic stability based on four-cycle *** addition,a mechanism study showed that superoxide radicals （·O2-）were the most important active species in the reaction *** production of H2O2was achieved through consecutive single-electron *** study deepens the understanding of the oxygen reduction reaction process and opens up a new venue for improving H2O2generation.

关键词： photocatalysis hydrogen peroxide oxygen reduction reaction potassium doping cyano group

Synergistically enhanced ORR and HER performance on Co-N-C coupled in-situ generated PtCo intermetallic

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Journal of Energy chemistry 2025年第1期100卷 721-729页

作者： Guanyu Luo Min Song Lulu An Xiao Huang Qian Zhang Chenhao Zhang Tao Shen Shuang Wang Deli Wang Key Laboratory of Material chemistry for Energy Conversion and Storage (Huazhong University of Science and Technology) Ministry of Education School of Chemistry and Chemical Engineering Huazhong University of Science and Technology

Integrating multi-scale sites in a composite catalyst is vital to realize efficient ***,a synergistic composite catalyst consisting of Co atomic sites and in-situ generated PtCo intermetallic compounds （IMCs）(o-PtCo@CoNC) is proposed through Co pre-anchoring and subsequent impregnation-reduction *** loading of Co atoms provides a chance for in-situ generating PtCo ordered intermetallic *** remaining Co single atoms and PtCo IMCs construct synergistic electrocatalytic *** from the ordered structure,synergistic effect of Pt Co IMCs and Co single atoms,o-PtCo@CoNC exhibits excellent electrocatalytic performance for oxygen reduction reaction （ORR） and hydrogen evolution reaction （HER） with mass activity of 1.21 A mgPt-1（at 0.9 V） and5.70 A mgPt-1（at an overpotential of 100 mV）,***,o-PtCo@CoNC delivers negligible loss of half-wave potential and overpotential during long-term stability test in acid solutions,with 13 mV decay after 50,000 potential cycles for ORR and a 2.7 mV decay after 20,000 potential cycles for *** integration strategy of single-atomic sites coupled IMCs paves the way for enhancing the activity and durability of Pt-based electrocatalysts.

关键词： Synergistic effect Intermetallics Single atomic sites Oxygen reduction reaction Hydrogen evolution reaction

Cobalamin-dependent radical S-adenosyl-L-methionine protein functions with a partner to successively methylate tricyclic indole alkaloid for chuangxinmycin maturation and derivatization

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Science China chemistry 2025年第1期68卷 308-316页

作者： Sili Wang Jiancheng Huang Yanan Du Wei Huang Yufeng Xue Xiaokun Xu Guannan Zhong Yuanyuan Shi Bin Hong Xiaoying Bian Wen Liu State Key Laboratory of Chemical biology Shanghai Institute of Organic Chemistry University of Chinese Academy of SciencesChinese Academy of Sciences State Key Laboratory of Microbial Technology Shandong University National Health Commission (NHC) Key Laboratory of Biotechnology for Microbial Drugs Institute of Medicinal BiotechnologyChinese Academy of Medical Science & Peking Union Medical College

Cobalamin(Cbl)-dependent radical S-adenosyl-L-methionine(SAM) proteins constitute the largest collection of the radical SAM superfamily that has hundreds of thousands of individual members. Many of these proteins are involved in the biosynthesis of pharmaceutically important natural products to catalyze chemically demanding reactions. In the biosynthetic pathway of chuangxinmycin(CXM), a unique indole alkaloid antibiotic with potent anti-infective activity, functionalization of the characteristic thiopyrano[4,3,2-cd]indole scaffold by regio-and stereoselective C3-methylation is believed to rely on a Cbl-dependent radical process, which, however, remained to be reconstituted biochemically. We here report the dissection of this enzymatic process, which requires the incorporation of Cxm8, a Cbl-dependent radical SAM protein, with Cxm9, a DUF5825family protein that shares no homology to any proteins of known functions. Cxm8 and Cxm9 function together by forming an unexpected heterodimeric complex that selectively catalyzes C3-methylation of the tricyclic indole-S-hetero ring system in a successive manner, achieving CXM and a recently identified, C3-dimethylated congener. Detailed biochemical characterization,isotope labeling, structural simulation and bioinformatics analysis rationalized the catalysis of the Cxm8/Cxm9 complex and particularly the necessity of the DUF5825 protein for C3-methylase activity. This is the first example that a Cbl-dependent protein acts with a partner to exhibit radical SAM activity.

关键词： cbl-dependent radical SAM protein biosynthesis chuangxinmycin stereoselective methylation

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： Nanorods

Intermolecular reductive coupling of aliphatic ketones with alkynes and alkenes by BCN photocatalysts

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Science China chemistry 2025年第1期68卷 181-185页

作者： Yanping Xia Luyang Sun Jiajia Cheng Sibo Wang Meifang Zheng Xinchen Wang State Key Laboratory of Photocatalysis on Energy and Environment College of Chemistry Fuzhou University

A photocatalytic process was developed for intermolecular reductive coupling of aliphatic ketones with alkynes/alkenes to furnish tertiary alcohols. Mechanistic studies support that boron carbonitrides(BCN) promote the single electron reduction of unactivated aliphatic ketones to generate ketyl radicals with visible light irradiation, which then react with alkynes and alkenes to afford the allylic and aliphatic alcohols, respectively. The heterogeneous photocatalytic system is compatible with diverse substrates including pharmaceutical-related molecules(43 examples) with reusability and scale-up experiments, verifying the complementary synthetic utility of this method to the homogeneous catalysts.

关键词： aliphatic ketones ketyl radical intermolecular cross-coupling tertiary alcohols

Atmospheric reductive catalytic fractionation of lignocellulose integrated with one-pot catalytic conversion of carbohydrate yielding valuable lignin monomers and platform chemicals from corn straw

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Green Energy & Environment 2025年第1期10卷 161-172页

作者： Meng-Ying Liu Zhe-Hui Zhang Xue-Qi Wang Qian Sun Chen Zhang Yu Li Zhuohua Sun Katalin Barta Feng Peng Tong-Qi Yuan State Key Laboratory of Efficient Production of Forest Resources Beijing Forestry UniversityBeijing100083China Beijing Key Laboratory of Lignocellulosic chemistry Beijing Forestry UniversityBeijing100083China Department of chemistry Organic and Bioorganic ChemistryUniversity of GrazHeinrichstrasse 28/II8010 GrazAustria

Developing a cost-effective and environmentally friendly process for the production of valuable chemicals from abundant herbal biomass receives great attentions in recent ***,taking advantage of the“lignin first”strategy,corn straw is converted to valuable chemicals including lignin monomers,furfural and 5-methoxymethylfurfural via a two steps *** key of this research lies in the development of a green and low-cost catalytic process utilizing magnetic Raney Ni catalyst and high boiling point ethylene *** utilization of neat ethylene glycol as the sole slovent under atmospheric conditions obviates the need for additional additives,thereby facilitating the entire process to be conducted in glass flasks and rendering it highly convenient for scaling *** the initial step,depolymerization of corn straw lignin resulted in a monomer yield of 18.1 wt%.Subsequently,in a dimethyl carbonate system,the carbohydrate component underwent complete conversion in a one-pot process,yielding furfural and 5-methoxymethylfurfural as the primary products with an impressive yield of 47.7%.

关键词： Atmospheric reductive catalytic fractionation Corn straw Ethylene glycol Raney Ni 5-Methoxymethylfurfural

Visible-light-responsive homologous heterostructure of oxynitrides constructed to boost charge separation and water splitting

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Science China chemistry 2025年第1期68卷 186-191页

作者： Hai Zou Yunfeng Bao Xueshang Xin Yu Qi Tengfeng Xie Fuxiang Zhang State Key Laboratory of Catalysis Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences School of chemistry and Chemical Engineering Liaoning Normal University College of chemistry Jilin University

Constructing type II heterostructures represents a widely recognized strategy for enhancing charge separation and photocatalytic efficiency,but it remains challenging to fabricate homologous heterostructures based on visible-light-responsive semiconductors,especially for popularly investigated （oxy）nitrides with low thermal ***,we synthesized a homologous heterostructure （denoted as YTON＿H） based on the oxynitrides of YTaO4-xNyand YTa *** heterostructure exhibits type II band structure alignment and intimate interface achieved through a magnesium （Mg） powder-assisted nitridation *** with widely reported heterologous heterostructures,the as-obtained YTON＿H homologous heterostructure could similarly exhibit enhanced charge separation as well as photocatalytic water splitting performance with respect to its counterparts(YTaO4-xNyand YTaON2).Meanwhile,detailed structural characterizations and spectroscopy analysis have been made to confirm the formation of heterostructure and promotion of spatial charge separation.

关键词： charge separation heterostructure oxynitride photocatalysis visible light

Deciphering Water Oxidation Catalysts:The Dominant Role of Surface chemistry over Reconstruction Degree in Activity Promotion

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Nano-Micro Letters 2025年第3期17卷 340-354页

作者： Li An Jianyi Li Yuanmiao Sun Jiamin Zhu Justin Zhu Yeow Seow Hong Zhang Nan Zhang Pinxian Xi * Zhichuan JXu Chun‑Hua Yan State Key Laboratory of Applied Organic chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu ProvinceFrontiers Science Center for Rare IsotopesCollege of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000People’s Republic of China School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798Singapore Faculty of Materials Science and Energy Engineering Institute of Technology for Carbon NeutralityShenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055People’s Republic of China Key Laboratory of Electromagnetic Materials and Devices National Center for International Research On Photoelectric and Energy MaterialsSchool of Materials and EnergyElectron Microscopy CenterYunnan UniversityKunming 650091People’s Republic of China State Key Laboratory of Baiyunobo Rare Earth Resource Researches and Comprehensive Utilization Baotou Research Institute of Rare EarthsBaotou 014030People’s Republic of China Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU‑HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryPeking UniversityBeijing 100871People’s Republic of China

Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution *** surface reconstruction has been widely observed in perovskite catalysts,and the reconstruction degree has been often correlated with the activity ***,a systematic study on the roles of Fe substitution in activation of perovskite LaNiO_(3)is *** substituting Fe content influences both current change tendency and surface reconstruction ***_(0.9)Fe_(0.1)O_(3)is found exhibiting a volcano-peak intrinsic activity in both pristine and reconstructed among all substituted perovskites in the LaNi_(1-x)Fe_(x)O_(3)(x=0.00,0.10,0.25,0.50,0.75,1.00)*** reconstructed LaNi_(0.9)Fe_(0.1)O_(3)shows a higher intrinsic activity than most reported NiFe-based ***,density functional theory calculations reveal that Fe substitution can lower the O 2p level,which thus stabilize lattice oxygen in LaNi0.9Fe0.1O3 and ensure its long-term ***,it is vital interesting that activity of the reconstructed catalysts relied more on the surface chemistry rather than the reconstruction *** effect of Fe on the degree of surface reconstruction of the perovskite is decoupled from that on its activity enhancement after surface *** finding showcases the importance to customize the surface chemistry of reconstructed catalysts for water oxidation.

关键词： Oxygen evolution reaction Perovskite oxides Doping Activation and reconstruction

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Facile synthesis of the dodecahydridododecaborate (B12H122-) from borane Lewis base adducts

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Science China chemistry 2025年

作者： Yi Jing Xin-Ran Liu Xing-Hua Wang Hui Han Sha-Sha Liang Xi-Meng Chen Dong-Hui Wei Lai-Sheng Wang Xue-Nian Chen College of chemistry Zhengzhou University School of chemistry and Chemical Engineering Henan Key Laboratory of Boron Chemistry and Advanced MaterialsHenan Normal University Department of chemistry Brown University

Polyhedral boranes are a class of well-known boron molecular clusters widely used in energy,chemistry,medicine,and materials science because of their unique physical and chemical *** efforts have been made in the past decades to find more effective synthetic methods for this important class of boron ***,existing synthetic methods suffer from low efficiency and low ***,we report a facile one-pot synthesis of[（CH3）3S]2B12H12with moderate yields at mild *** mechanisms for the multi-step chemoselective synthesis of B12H122-without other by-products are elucidated based on theoretical results and our previous *** Lewis base used in B–H bond condensation reaction,which acts as a hydrogen or to balance the newly generated polyhedral borane charges,is proposed and studied in *** current study has led to a more effective and selective synthetic method for B12H122-and has also implicated the syntheses of other new polyhedral boranes.

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