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Enantioselective reductive conjugate alkenylation of α,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 Engineering Lanzhou University

Reactions involving alkenyl acetates offer cost-effective and environmentally friendly routes for alkene synthesis, yet their asymmetric variant remains elusive. Concurrently, asymmetric conjugate alkenylation predominantly centered on nucleophilic addition using alkenyl–M. This manuscript presents an asymmetric reductive conjugate alkenylation reaction involving alkenyl acetates. The method facilitates the enantioselective addition of keto alkenyl groups to α,β-enones, resulting in the formation of unsaturated diketones—a class of useful structural motifs that are challenging to access otherwise. The 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

Research progress of catalysts for direct coal liquefaction

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Journal of Energy chemistry 2025年第1期100卷 481-497页

作者： Wei Song Penggao Liu Xinyue Chen Ting Wang Chunrong He Rui Hao Kaiyu Liu State Key Laboratory of chemistry and Utilization of Carbon Based Energy Resources College of Chemistry Xinjiang University college of chemistry and chemical engineering Henan Polytechnic University Hunan Provincial Key Laboratory of chemical Power Sources College of Chemistry and Chemical Engineering Central South University

Coal direct liquefaction technology is a crucial contemporary coal chemical technology for efficient and clean use of coal resources. The development of direct coal liquefaction technology and the promotion of alternative energy sources are important measures to guarantee energy security and economic security. However, several challenges need to be addressed, including low conversion rate, inadequate oil yield, significant coking, demanding reaction conditions, and high energy consumption. Extensive research has been conducted on these issues, but further exploration is required in certain aspects such as pyrolysis of macromolecules during the liquefaction process, hydrogen activation, catalysts' performance and stability, solvent hydrogenation, as well as interactions between free radicals to understand their mechanisms better. This paper presents a comprehensive analysis of the design strategy for efficient catalysts in coal liquefaction, encompassing the mechanism of coal liquefaction, catalyst construction,and enhancement of catalytic conversion efficiency. It serves as a comprehensive guide for further research endeavors. Firstly, it systematically summarizes the conversion mechanism of direct coal liquefaction, provides detailed descriptions of various catalyst design strategies, and especially outlines the catalytic mechanism. Furthermore, it addresses the challenges and prospects associated with constructing efficient catalysts for direct coal liquefaction based on an understanding of their action mechanisms.

关键词： Direct coal liquefaction Catalysts Mechanism of action Solvent hydrogenation

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 Engineering Lanzhou University School of chemistry and chemical engineering Shanghai Jiao Tong University School of Biotechnology and Health Sciences Wuyi University

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 enantioselectivities. Furthermore, 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

CO2-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 Engineering Tsinghua University college of chemistry and Molecular engineering Peking University Ordos Laboratory

Renewable energy-driven bicarbonate conversion to valuable chemicals presents an attractive strategy for mitigating CO2emissions,as bicarbonate can be efficiently generated from the capture of atmospheric CO2using alkaline solutions with reactive *** this work,we present a CO2-mediated bicarbonate conversion to pure formate using a cation exchange membrane-based electrolyzer with a 25 cm2electrode *** 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

Dual modulation of homogeneous nanomaterialization and electrochemical activation enhancing zinc ion storage

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Science China chemistry 2025年第1期68卷 385-393页

作者： Jianwei Wang Huan Wang Kangning Wang Wenhui Wang Wenlin Zhang Yanzhong Zhen School of chemistry & chemical engineering Yan'an University

Vanadium-based electrode materials are widely investigated,but the low specific capacity and slow electrochemical kinetics in aqueous zinc-ion batteries still limit their commercial ***,the VS2/Ca V4O9material with the morphology of nanoflower was synthesized by a one-step hydrothermal *** to the blocky structure of pure VS2material,the VS2/Ca V4O9material is composed of thinner homogeneous *** open structures could provide abundant electrochemical active sites and ion transport channels,and then promote the electrochemical reaction *** addition,they can also buffer the bulk strain during the reaction *** improve the utilization of vanadium elements,an in-situ electrochemical activation strategy is used to explore the storage performance of the VS2/Ca V4O9material,the different activation voltage range of 0.4–1.6 and 0.4–1.4 V are selected,*** with the longer activation plateau of activated-VS2,the VS2/Ca V4O9cathode could quickly reach the activation state in the range of 1.4–1.6 V and cause the release of additional Zn storage sites *** VS2/Ca V4O9cathode delivers a higher power density of 37,000 W kg-1and a significant energy density of 423 Wh *** the high current density of 15 A g-1,the VS2/Ca V4O9cathode still has a discharge capacity of 183.9m Ah g-1after 5,000 cycles,and the capacity decay rate per cycle is only 0.0042%.Continuous cyclic voltammetry （CV） curves,electrochemical impedance spectroscopy （EIS） measurements,density functional theory （DFT） calculation and galvanostatic intermittent titration technique （GITT） measurements demonstrate that the VS2/Ca V4O9cathode has a faster ion diffusion/charge transfer ***,the assembled flexible device has an excellent mechanical stability.

关键词： dual modulation homogeneous nanomaterialization electrochemical activation zinc ion storage

CaH2-promoted activity of Ni-carbonate interface for CO2 methanation

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Journal of Energy chemistry 2025年第1期100卷 522-532页

作者： Jin-Peng Wang Guo-Cui Mao Hui-Lin Jiang Bao-Xia Dong Yun-Lei Teng School of chemistry and chemical engineering Yangzhou University

Transition metal-carbonate interfaces often act as active sites in heterogeneous catalytic *** interface between transition metal and metal carbonate exhibits a dynamic equilibrium during the CO2hydrogenation reaction,involving surface carbonate hydrogenation and ***,there have been few reports on engineering the activity of the interface between transition metal and alkaline earth metal carbonate for catalytic *** work demonstrated that the incorporation of CaH2in Ni/CaCO3enhances the CO2methanation activity of the *** CO2conversion for Ni/CaH2-CaCO3reached 68.5%at 400°C,which was much higher than that of the Ni/CaCO3（31.6%） and Ni/CaH2-CaO （42.4%） ***,the Ni/CaH2-CaCO3catalysts remained stable during the stability test for 24 h at 400°C and 8 *** research revealed that CaH2played a crucial role in promoting the activity of the Ni-carbonate interface for ***2could modify the electronic structure of Ni and tune the structural properties of CaCO3to generate medium basic sites （OH groups）,which are favorable for the activation of H2and ***-situ Fourier transform infrared spectroscopy （FTIR） analysis combined with density functional theory calculations demonstrated that CO2activation occurs at the hydroxyl group （OH） on the CaH2-modified Ni-carbonate surface,leading to the formation of CO3H****,our study has confirmed that CO2methanation over the Ni/CaH2-CaCO3catalysts proceeds via the formate pathway.

关键词： CO 2 methanation Metal hydride Ni catalysts Carbonate Metal-carbonate interface

High‑Entropy Electrode Materials:Synthesis,Properties and Outlook

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Nano-Micro Letters 2025年第1期17卷 472-506页

作者： Dongxiao Li Chang Liu Shusheng Tao Jieming Cai Biao Zhong Jie Li Wentao Deng Hongshuai Hou Guoqiang Zou Xiaobo Ji college of chemistry and chemical engineering Central South UniversityChangsha 410083People’s Republic of China School of chemistry and chemical engineering Hunan Institute of EngineeringXiangtan 411104People’s Republic of China

High-entropy materials represent a new category of high-performance materials,first proposed in 2004 and extensively investigated by researchers over the past two *** definition of high-entropy materials has continuously *** the last ten years,the discovery of an increasing number of high-entropy materials has led to significant advancements in their utilization in energy storage,electrocatalysis,and related domains,accompanied by a rise in techniques for fabricating high-entropy electrode ***,the research emphasis has shifted from solely improving the performance of high-entropy materials toward exploring their reaction mechanisms and adopting cleaner preparation ***,the current definition of high-entropy materials remains relatively vague,and the preparation method of high-entropy materials is based on the preparation method of single metal/low-or medium-entropy *** should be noted that not all methods applicable to single metal/low-or medium-entropy materials can be directly applied to high-entropy *** this review,the definition and development of high-entropy materials are briefly ***,the classification of high-entropy electrode materials is presented,followed by a discussion of their applications in energy storage and catalysis from the perspective of synthesis ***,an evaluation of the advantages and disadvantages of various synthesis methods in the production process of different high-entropy materials is provided,along with a proposal for potential future development directions for high-entropy materials.

关键词： High-entropy Energy storage Electrode materials

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Transforming waste particles into valuable adsorbents via amyloid-mediated molecular engineering

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Science China chemistry 2025年第1期68卷 317-328页

作者： Qingmin Yang Jian Zhao Yujia Zhang Xingyu Zhou Hao Ren Bowen Hu Zhongli Lei Lixin Chen Peng Yang School of Material and chemical engineering Bengbu University Anhui Provincial engineering Laboratory of Silicon-Based Materials School of chemistry and chemical engineering Northwestern Polytechnical University Key Laboratory of Applied Surface and Colloid chemistry Ministry of Education School of Chemistry and Chemical EngineeringShaanxi Normal University Xi'an Key Laboratory of Polymeric Soft Matter School of Chemistry and Chemical Engineering Shaanxi Normal University International Joint Research Center on Functional Fiber and Soft Smart Textile School of Chemistry and Chemical EngineeringShaanxi Normal University

The high-value utilization of industrial solid waste using a facile and eco-friendly process is of great interest and significance in reducing environmental pollution and developing a green circular economy. Herein, we propose an amyloid-mediated molecular engineering strategy to transform particulate waste into valuable adsorbents for metal ions. Our method has the advantage of aqueous solution fabrication under mild conditions without the use of high-temperature hydrothermal methods and toxic chemical reagents. Amyloid-mediated molecular engineering manipulates the phase transition of bovine serum albumin(BSA)on particulate waste surfaces, resulting in a remarkable ～3.1 times improvement in the adsorption capacity of fly ash, a typical industrial solid waste for gold ions after modification with the phase-transitioned BSA(PTB). The resultant adsorption ability was 69–1,980 times higher than those of conventional and emerging adsorbent materials such as ion exchange resins, activated carbon(AC), covalent organic frameworks(COFs), and metal-organic frameworks(MOFs). We further demonstrated the application of our PTB-modified materials in the recovery of precious metals from low-grade gold ore and electronic waste leachates. Consequently, this strategy could increase the value of waste materials nearly 27 times. In addition, this method is generally extendable to other conventional industrial adsorbents such as resin, clay, and Al2O3, and enhances their adsorption capabilities at least twofold. Overall, this work provides a simple and green approach for improving the adsorption performance of solid particles, and is expected to develop into a universal strategy for transforming waste particles into high-value-added products.

关键词： amyloid-like protein aggregates surface engineering fly ash solid waste adsorption

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