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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 Engineering School of Materials and Energy Lanzhou University College of chemistry and chemical engineering Luoyang Normal University

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）2after 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-1and long-term durability (over1270 h at 10 m A cm-2and 110 h at 200 mA cm-2).This work presents a new perspective on designing highly efficient OER electrocatalysts.

关键词： X ray photoelectron spectroscopy

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

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

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

High-temperature-tolerant flexible supercapacitors: Gel polymer electrolytes and electrode materials

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Journal of Energy chemistry 2025年第1期100卷 426-457页

作者： Chong Peng Xinyi Huang Mingwei Zhao Shuling Liao Quanhong Yang Nianjun Yang Siyu Yu School of chemistry & chemical engineering Southwest University Nanoyang Group Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage School of Chemical Engineering and Technology and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Tianjin University department of chemistry & IMO-IMOMEC Hasselt University

The development of flexible supercapacitors(FSCs) capable of operating at high temperatures is crucial for expanding the application areas and operating conditions of supercapacitors. Gel polymer electrolytes and electrode materials stand as two key components that significantly impact the efficacy of hightemperature-tolerant FSCs(HT-FSCs). They should not only exhibit high electrochemical performance and excellent flexibility, but also withstand intense thermal stress. Considerable efforts have been devoted to enhancing their thermal stability while maintaining high electrochemical and mechanical performance. In this review, the fundamentals of HT-FSCs are outlined. A comprehensive overview of state-of-the-art progress and achievements in HT-FSCs, with a focus on thermally stable gel polymer electrolytes and electrode materials is provided. Finally, challenges and future perspectives regarding HT-FSCs are discussed, alongside strategies for elevating operational temperatures and *** review offers both theoretical foundations and practical guidelines for designing and manufacturing HT-FSCs, further promoting their widespread adoption across diverse fields.

关键词： Polymer membrane electrodes

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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Maximizing biomass utilization: An integrated strategy for coproducing multiple chemicals

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Journal of Energy chemistry 2025年第1期100卷 180-191页

作者： Byeongchan Ahn Sua Jo Jonggeol Na J.Jay Liu Young-Ju Kim Wangyun Won department of chemical and Biological engineering Korea University department of chemical engineering (Integrated process) Kyung Hee University department of chemical engineering and Materials Science Ewha Womans University department of chemical engineering Pukyong National University Resources engineering Plant Research department Korea Institute of Geoscience and Mineral Resources

Lignocellulosic biomass is one of the viable solutions to alleviate the global warming. However, the limited utilization of biomass majorly focused on cellulose and hemicellulose restricts the economic and environmental feasibilities. To cope with this issue, we proposed an integrated process of co-producing 1,6-hexanediol（1,6-HDO） with tetrahydrofuran and adipic acid from biomass, referred to as Strategy A. To compare the impacts of lignin upgrading and feedstock, Strategy B, which co-produces tetrahydrofuran alone, and Strategy C, which is the traditional route to produce 1,6-HDO from fossil fuels, were used. Heat networks are also designed to reduce operating costs and indirect carbon emissions due to energy consumption, saving 87% and 83% of the heat and cooling requirements, respectively, in Strategy A. The market competitiveness of Strategy A was evaluated by determining the minimum selling price through techno-economic analysis, and sustainability was thoroughly investigated by quantifying the environmental impacts through both midpoint and endpoint life-cycle assessments（LCAs）.Strategy A was found to be the most favorable both economically（USRDSCHARDOLLAR3,402/ton） and environmentally（-26.9 kg CO2eq.）. This indicates that lignin valorization is not only economically but also environmentally preferred. Finally, changes in economic and environmental feasibilities depending on economic, process, and environmental parameters were investigated using sensitivity and uncertainty analyses. The results of these analyses provide valuable insight into bio-based chemical production.

关键词： Carbon capture and utilization

Modular assembly of complex C-alkyl glycoside enabled via cooperative NHC and photoredox catalysis

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Science China chemistry 2025年

作者： Rui-Qiang Jiao Ming Li Xi Chen Mei-Ze Xu Tian Ding Xiao-Ping Gong Zhuo-Mei Li Xue-Yuan Liu Yong-Min Liang State Key Laboratory of applied Organic chemistry Lanzhou University College of chemistry and chemical engineering Northwest Normal University

C-Alkyl glycosides are found in natural products and are indispensable in drug development programs,owing to their diverse range of medicinal ***-component reactions involving glycosyl radical addition are well documented and proved efficient for the C-alkyl glycosides ***,multicomponent reactions for the rapid and controllable construction of structurally diversified C-alkyl glycosides in a single step remains a significant challenge due to the issues associated with balancing reactivity,compatibility,and ***,we report an NHC and photoredox co-catalyzed three-component method to access complex and valuable C-alkyl *** protocol exhibits broad substrate scope and excellent chemoand ***,nine types of sugars are compatible with this *** addition,the generality of this catalytic strategy was further highlighted by the potential for scalable production,the feasibility of further modifications of the products and its successful application in the late-stage functionalization of pharmaceutical skeletons.

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Establishing a new testing protocol of the electrochemical stability window for electric double-layer capacitors

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Science China chemistry 2025年第1期68卷 217-225页

作者： Ruilin Hou Xiaoxi Zhao Tingting Liang Qingyun Dou Shan Xu Xingbin Yan School of Materials Science and engineering Sun Yat-sen University Laboratory of Clean Energy chemistry and Materials Lanzhou Institute of Chemical Physics Chinese Academy of Sciences College of engineering and applied Sciences Nanjing University Center of Industrial Analysis and Testing Guangdong Academy of Science

The electrochemical stability window(ESW) is crucial for determining the energy density of electric double-layer capacitors(EDLCs). However, current ESW testing protocols of EDLCs are strongly affected by artificial factors, thereby leading to unreliable result. To solve this problem, we first identify the key shortcomings of the traditional protocols by analyzing their test principles. Subsequently, taking an aqueous carbon-based EDLC as an example, we design a side reaction descriptor to represent the response difference in the charging capacitance to side reactions between the cyclic voltammetry and galvanostatic chargedischarge methods. With the aid of this descriptor, we propose a new ESW testing protocol, which is not only able to completely avoid the adverse influence of subjective factors but also fully consider the operating condition limitations. The protocol can be extended from the single electrode to the full device. This work proposes a more rigorous definition of ESW and provides a reliable protocol for evaluating the ESW of EDLCs.

关键词： electric double-layer capacitors electrochemical stability window testing protocol side reaction descriptor operating limitation