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Deciphering the role of ultra-low-loaded rhodium in NiFe-MIL-53 for superior oxygen evolution reaction

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Journal of Energy chemistry 2025年第1期100卷 77-86页

作者： Jinzhi Jia Jinhua Zhang Kailu Guo Lanyue Zhang Gening Du Hao You Junfeng Huang Mudong Tu Hua Li Yong Peng Wei Dou Cailing Xu state key laboratory of applied organic chemistry College of Chemistry and Chemical EngineeringSchool of Materials and EnergyLanzhou UniversityLanzhou 730000GansuChina College of chemistry and Chemical Engineering Luoyang Normal UniversityLuoyang 471934HenanChina

Designing highly active and stable electrocatalysts of oxygen evolution reaction(OER)is one of the crucial *** this study,a novel OER electrocatalyst,NiFe-MIL-53 modified with ultra-low rhodium(Rh@NiFe-MIL-53),is successfully prepared via the hydrothermal ***-situ Raman spectroscopy and electrochemical impedance spectroscopy reveal that the doped Rh accelerates the phase transformation of NiFe-MIL-53 and the in-situ formed Rh@NiFeOOH is the actual active *** importantly,the enhanced reversibility of electrochemical reconstruction between NiFeOOH and NiFe(OH)_(2)after doping Rh is beneficial for improving the electrochemical stability of the catalyst.X-ray photoelectron spectroscopy spectra show the strong electronic interaction between single-atom Rh and Ni/Fe in Rh@***,theoretical calculations confirm that the integration of single-atom Rh into the NiFeOOH successfully reduces the band gap,regulates the d-band center(εd),accelerates the charge transfer,and optimizes the adsorption behavior of oxygen-containing intermediates,thereby lowering the energy barrier of rate-determining ***,the optimized Rh@NiFe-MIL-53 exhibits excellent OER activity(240 mV)with a small Tafel slope of 48.2 mV dec^(-1)and long-term durability(over1270 h at 10 m A cm^(-2)and 110 h at 200 mA cm^(-2)).This work presents a new perspective on designing highly efficient OER electrocatalysts.

关键词： NiFe-MIL-53 Rh Electrochemical reconstruction Catalytic mechanism Oxygen evolution reaction

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

Improvement of charge-transfer kinetics via MXene and cobalt containing polyoxometalate loading on CdS for photocatalytic hydrogen production

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Science China chemistry 2025年第2期68卷 772-780页

作者： Yu Feng Xiao Fang Jinnuo Zang Bin Song Chunlian Hu Xiaoyu Dong Yong Ding state key laboratory of applied organic chemistry Key Laboratory of Advanced Catalysis of Gansu ProvinceCollege of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China state key laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization State Key Laboratory for Oxo Synthesis and Selective OxidationLanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China

Hydrogen is a renewable and clean energy,and photocatalytic water splitting for hydrogen evolution technology is a promising technical means to solve the development *** this study,the ternary composite Co_(8)POM@MXene–CdS hybrid catalyst was constructed and used for photocatalytic hydrogen *** the condition of AM 1.5G simulated sunlight,the photocatalytic H_(2) evolution rate of the ternary composite was 8.13 mmol g^(−1) h^(−1),which was more than 25 times higher than that of the bare *** means of synchronous illumination X-ray photoelectron spectroscopy(SI-XPS)and density functional theory(DFT)calculations,it was proved that the loading of MXene and Co_(8)POM improved the photogenerated carrier separation and immigration efficiency on *** photogenerated electrons transfer from CdS to ***_(8)POM containing the{Co_(4)O_(3)}quasi-cubane,as an oxidation co-catalyst,accepts photogenerated holes from CdS to catalyze the oxidation reaction of TEOA,which improves the photocatalytic hydrogen production activity and the stability of CdS.

关键词： CdS polyoxometalates MXene hybrid catalyst photocatalytic hydrogen evolution

Tandem asymmetric dearomatized functionalization reaction of phenols with Evans-ynamides enabled by divergent electrophiles

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Science China chemistry 2025年第2期68卷 649-660页

作者： Ying-Qi Zhang Gan-Lu Qian Yun Liu Jia-Hui Li Xin Hong Zhou Xu Bo Zhou Long-Wu Ye state key laboratory of Physical chemistry of Solid Surfaces Key Laboratory of Chemical Biology of Fujian Provinceand College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Center of chemistry for Frontier Technologies Department of ChemistryState Key Laboratory of Clean Energy UtilizationZhejiang UniversityHangzhou 310027China Jiangsu key laboratory of New Drug Research and Clinical Pharmacy School of PharmacyXuzhou Medical UniversityXuzhou 221004China state key laboratory of Elemento-organic chemistry Nankai UniversityTianjin 300071China state key laboratory of Organometallic chemistry Chinese Academy of SciencesShanghai 200032China

Herein,we disclose a highly regio-/chemoselective tandem asymmetric dearomatized halofunctionalization reaction of phenoltethered ynamides with diverse electrophilic halogenation sources in a catalyst-free manner for the practical and rapid assembly of a series of halogenated spirocyclic ***,the related dearomatized selenation and protonation are also achieved,affording the corresponding selenated and protonated spirocycles in high ***,the enantioselectivities of these products can be perfectly induced by Evans auxiliaries(99%ees).Significantly,this protocol not only represents the first tandem asymmetric halofunctionalization reaction of phenol derivatives,but also constitutes the first asymmetric halogenation/selenation of *** calculations indicate a remote induction model of Evans chiral auxiliary-attached keteniminium.

关键词： alkynes cyclization dearomatization Evans chiral auxiliary spirocycles

Trifluoromethylative homo-coupling of carbonyl compounds

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Chinese Chemical Letters 2025年第1期36卷 283-287页

作者： Xinlong Han Huiying Zeng Chao-Jun Li The state key laboratory of applied organic chemistry Lanzhou UniversityLanzhou 730000China department of chemistry FQRNT Centre for Green Chemistry and CatalysisMcGill UniversityMontrealQuebecH3A 0B8Canada

Carbonyl compounds are abundant in nature and represent a substantial portion of biomass *** significant recent progress in homo-coupling of carbonyl compounds,achieving their deoxyfunctionalization homo-coupling remains a highly intricate ***,we report an entirely novel reaction paradigm:the trifluoromethylative homo-coupling of carbonyl compounds via hydrazones,which enables the formation of three C(sp^(3))-C(sp^(3))bonds in a single *** method provides a new pathway for synthesizing trifluoromethylative coupling product which has unique applications in both fields of medical and material *** investigations have unveiled that the formation of a trifluoromethyl-substituted benzyl radical plays a pivotal role as a key intermediate in this reaction.

关键词： Carbonyl compounds Trifluoromethylation Homo-coupling C(sp^(3))-C(sp^(3))bond formation

Trinuclear gold-catalyzed site-selective alkylation of peptides

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Science China chemistry 2025年第1期68卷 249-256页

作者： Qing-Yun Fang Chengyihan Gu Yinghan Chen Wencheng Yan Yong Liang Weipeng Li Chengjian Zhu Jie Han Jin Xie state key laboratory of Coordination chemistry Jiangsu Key Laboratory of Advanced Organic MaterialsChemistry and Biomedicine Innovation Center(ChemBIC)School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China Green Catalysis Center College of ChemistryZhengzhou UniversityZhengzhou 450001China state key laboratory of Natural Medicines China Pharmaceutical UniversityNanjing 211198China

Selective modification of peptides has always been a challenging *** selective alkylation of peptides can alter the biological activity and physical properties of molecules,and it has gained significant research *** herein disclose an intriguing gold-catalyzed alkylation of peptides using bench-stable unactivated alkyl bromides under photoredox catalysis.A wide range of structurally diverse primary,secondary and tertiary alkyl bromides serve as effective coupling partners to precisely connect with theα-C(sp^(3))–H in glycine residue of *** protocol demonstrates an exceptionally broad scope for alkyl halides and excellent tolerance for a wide range of useful functional groups.A series of relay transformations to construct cyclic peptides,to proceed click reaction and to realize peptide fluorescence labeling further enhance its synthetic *** addition,mechanistic studies and density functional theory(DFT)calculations reveal an inner-sphere and subsequent outersphere single electron transfer(SET)mechanism.

关键词： gold catalysis peptide alkylation C-C coupling radical

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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

Microdynamic modulation through Pt–O–Ni proton and electron “superhighway” for pH-universal hydrogen evolution

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Journal of Energy chemistry 2025年第2期101卷 808-815页

作者： Dewen Wang Yuting Chen Bohan Yao Tian Meng Yanchao Xu Dongxu Jiao Zhicai Xing Xiurong Yang state key laboratory of Electroanalytical chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences University of Science and Technology of China department of chemistry Shenzhen Grubbs Institute and Guangdong Provincial Key Laboratory of Energy Materials for Electric Power Southern University of Science and Technology state key laboratory of Automotive Simulation and Control School of Materials Science and Engineering Jilin University

Optimizing the microdynamics in alkaline and neutral conditions is a significant but challenging task in developing pH-universal hydrogen evolution（HER） ***,a unique Pt-O-Ni bridge has been constructed to alter the coordination and electronic environment between Pt nanoparticles（Pt_n）and nickel metaphosphate（NPO） substrate（Pt-NPO）.Sufficient electron transfer from NPO to Pt_n to maintain an electron-rich environment and a low valence state of Pt_***,H*is produced from the H2O dissociation on Ni site and then spillover toward Pt sites to bind into H2,which makes up for the insufficient H2O dissociation ability of Pt in Volmer ***-NPO exhibits long-term stability and only need the overpotentials of 22.3,33.0 and 30.5 mV to attain 10 mA cm-2in alkaline,neutral and acidic media,*** anion-exchange membrane（AEM） water electrolyzer catalyzed by Pt-NPO shows high water electrolysis performance that a cell voltage of 1.73 V is needed to obtain the current density of500 mA cm-2in 1 M KOH at 80℃,at the same time maintains good stability for 350 *** regulation strategy proposed in this work is helpful for the design and synthesis of highly efficient pH-universal HER electrocatalysts.

关键词： Atomic and electronic regulation Hydrogen evolution reactions Metal-support interactions Microdynamics pH-universal HER electrocatalysts

De novo synthesis of atropisomeric benzofurans via Cu/SPDO complex catalyzed asymmetric formal[3+2]annulation

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Science China chemistry 2025年第1期68卷 174-180页

作者： Fan-Xiao Meng Xing-Yu Wang Ka Lu Ju-Song Yang Fu-Min Zhang Ai-Jun Ma Bao Du Yong-Qiang Tu state key laboratory of applied organic chemistry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China School of chemistry and Chemical Engineering Shanghai Jiao Tong UniversityShanghai 200240China School of Biotechnology and Health Sciences Wuyi UniversityJiangmen 529020China

Herein,the de novo synthesis of atropisomeric benzofurans through the Cu/spirocyclic-pyrrolidine-oxazoline(SPDO)complex catalyze asymmetric formal[3+2]cycloaddition between quinones and ynamides is explored,producing a range of structurally diverse axially chiral benzofurans in satisfactory yields with good to excellent ***,density functional theory calculations were applied to explain the possible reaction mechanism.

关键词： benzofuran atropisomers novel de novo synthetic strategy asymmetric formal[3+2]cycladdition Cu/SPDO complex DFT calculations