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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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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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Potassium ions and cyano group modified g-C_(3)N_(4) for effective generation of H_(2)O_(2) 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 UniversityChengdu 610106China department of chemistry and Biochemistry University of CaliforniaSanta CruzCA 95064USA

Potassium ions(K^(+))doped graphitic carbon nitride(g-C_(3)N_(4))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(H_(2)O_(2))generation rate of2,140.2μmol h^(-1)g^(-1).The 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-C_(3)N_(4)layers,which enhanced charge transfer ***,the cyano group enhanced the adsorption capacity of protons(H^(+))and promoted the yield of H_(2)O_(2).The catalyst exhibited excellent photocatalytic stability based on four-cycle *** addition,a mechanism study showed that superoxide radicals(·O_(2)^(-))were the most important active species in the reaction *** production of H_(2)O_(2)was achieved through consecutive single-electron *** study deepens the understanding of the oxygen reduction reaction process and opens up a new venue for improving H_(2)O_(2)generation.

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

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Investigation on Cu promotion effect on Ce-based solid solution-anchored Rh single atoms for three-way catalysis

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Chinese Chemical Letters 2025年第2期36卷 574-578页

作者： Jianing He Xiao Wang Zijian Wang Ruize Jiang Ke Wang Rui Zhang Huilin Wang Baokang Geng Hongyi Gao Shuyan Song Hongjie Zhang State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied Chemistry Chinese Academy of Sciences School of Applied chemistry and Engineering University of Science and Technology of China China School of Materials Science and Engineering University of Science and Technology Beijing department of chemistry Tsinghua University

The three-way catalyst（TWC）, as a promising approach to control automobile exhaust emission, has been widely studied and applied. However, it still suffers from the high light-off temperature and poor ***, we synthesized a multicomponent catalyst Rh/Cu-CeSn by using Cu metal doping to modify the Ce-based solid solution, which exhibited good TWC catalytic performance: the light-off temperatures for CO, NO, and C3H6conversion are 172 ℃, 266 ℃, and 193 ℃, respectively. Moreover, the catalyst still maintained good activity after 12 h of the continuous reaction under high-temperature conditions. The experiments and mechanism studies reveal that due to the redox pair Cu+/Cu2+, the Cu incorporation can effectively inhibit the Rh transition to the oxidation state and greatly enhance the catalytic activity and stability. This work provides a viable strategy for precise characteristic modulation of composite oxide supports during the fabrication of noble metal-based catalysts, which significantly reduces environmental pollution from energy applications.

关键词： Co-precipitation Oxygen vacancies Rhodium (Rh) catalyst Solid solution Three-way catalysts (TWC)

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Ultrastrong MXene films for bone regeneration

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Science China Materials 2025年

作者： Jinghong Li department of chemistry Center for Bioanalytical Chemistry Key Laboratory of Bioorganic Phosphorus Chemistry and Chemical Biology (Ministry of Education) Tsinghua University

Guided bone regeneration (GBR),as an important clinical treatment of bone defects,has long been a great challenge in modern *** addition to biological scaffolds,growth factors,and stem cells,barrier membranes for GBR application also play a key role in preventing the invasion of cells from the surrounding epithelium and connective tissue[1–3],to favor osteoprogenitor cells to proliferate and form new bone tissue in the site of *** commercial GBR membranes,such as polytetrafluoroethylene,titanium,collagen,and polyesters,exhibit low osteogenesis performance because of the lack of suitable antioxidant ability.

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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

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Biopolymer Decorated Pencil Graphite Electrode for the In-situ Quantification of L-Tryptophan in Dietary Supplements

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Journal of Analysis and Testing 2025年第01期 82-95页

作者： V.Devika P.J.Sreelekshmi B.Vedhanarayanan Sandhya Sadanandan R.Rejithamol department of chemistry Amrita Vishwa Vidyapeetham Graduate School of Science Chiba University department of chemistry School of Advanced SciencesVIT-AP University

A simplistic and novel electrochemical sensor for selectively detecting the essential amino acid tryptophan in dietary supplements was fabricated on a pencil graphite electrode modified with a tryptophan-based dipeptide. The dipeptide was synthesized using common synthetic strategy for amino acid couplings. The modified electrode was characterized by scanning electron microscopy, impedance spectroscopy, cyclic voltammetry, and infrared spectroscopy. Differential pulse voltammetry was used to study the electrochemical response of the fabricated electrode to tryptophan in dietary supplements. Under the optimized experimental conditions, a distinct oxidation peak at + 0.671 V corresponding to tryptophan was noticed in differential pulse voltammetry, which indicated the detection of tryptophan by the fabricated electrode. The oxidation peak current for tryptophan was found to be linear within a concentration range of 10–350 μM with a lower detection limit of 1.2 μM, and the sensitivity of the fabricated electrode was 6.9 μA/μM/cm 2. Excellent selectivity, permissible reproducibility, and good stability of the sensor make it undoubtedly suitable for determining tryptophan in dietary supplements.

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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

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Phenyl-extended resorcin[4]arene opens up a new avenue for highly efficient iodine adsorption

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Science China chemistry 2025年第2期 405-406页

作者： Jingyu Chen Jiong Zhou department of chemistry College of SciencesNortheastern University

Macrocyclic arenes have become an important tool in supramolecular chemistry due to their special structure, easy functionalization and prominent host–guest properties. The design and synthesis of macrocyclic arenes with novel structures and excellent performances have been the focus of research in the field of supramolecular chemistry, including calixarenes, pillararenes, biphenarenes, and hybridarenes[1].

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Visualizing charge transfer and nuclear quantum effects in the hydrogen bond network of water

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Science China chemistry 2025年第03期 810-811页

作者： Ying Gao Haotian Wang Bin Zhang department of chemistry School of ScienceTianjin University

Water,one of the most common and important solvents on earth,is widely used in biology,physics,chemistry,and other fields [1].The hydrogen bond interactions between water molecules form a highly dynamic and synergistic network[2],which plays a key role in the properties of *** electron charge transfer and nuclear quantum effect(NQE)are important factors affecting the stability and structure of hydrogen bond networks [3],directly influencing water-involved biological and chemical processes.

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