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Identifying the dynamic behaviors in complete reconstruction of Co-based complex precatalysts during electrocatalytic oxygen evolution

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Journal of Energy chemistry 2025年第1期100卷 226-233页

作者： Jingfang Zhang Danyang Wu Linke Cai Youluan Lu Fanpeng Cheng Lijuan Shi Qun Yi Yao Liu Yi Huang key laboratory of Green Chemical Engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education Hubei Key Laboratory of Novel Reactor and Green Chemical Technology School of Chemical Engineering & Pharmacy Wuhan Institute of Technology key laboratory of Pesticide & Chemical biology of Ministry of Education Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of Education College of Chemistry Central China Normal University College of Materials Science and Engineering Fuzhou University

Transition metal-based nanomaterials have emerged as promising electrocatalysts for oxygen evolution reaction（OER）. Considerable research efforts have shown that self-reconstruction occurs on these nanomaterials under operating conditions of OER process. However, most of them undergo incomplete reconstruction with limited thickness of reconstruction layer, leading to low component utilization and arduous exploration of real catalytic mechanism. Herein, we identify the dynamic behaviors in complete reconstruction of Co-based complexes during OER. The hollow phytic acid（PA） cross-linked CoFe-based complex nanoboxes with porous nanowalls are designed because of their good electrolyte penetration and mass transport ability, in favor of the fast and complete reconstruction. A series of experiment characterizations demonstrate that the reconstruction process includes the fast substitution of PA by OH-to form Co（Fe）(OH)xand subsequent potential-driven oxidation to Co（Fe）OOH. The obtained CoFeOOH delivers a low overpotential of 290 mV at a current density of 10 mA cm-2and a long-term *** experiment results together with theory calculations reveal that the Fe incorporation can result in the electron rearrangement of reconstructed CoFeOOH and optimization of their electronic structure,accounting for the enhanced OER activity. The work provides new insights into complete reconstruction of metal-based complexes during OER and offers guidelines for rational design of high-performance electrocatalysts.

关键词： Complete reconstruction Co-based complex Precatalysts Oxygen evolution reaction

Engineering atomic Rb-N configurations to tune radical pathways for highly selective photocatalytic H2O2 synthesis coupled with biomass valorization

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Journal of Energy chemistry 2025年第1期100卷 215-225页

作者： Jiaye Li Shuang Pan Yihuang Chen Qiong Liu College of chemistry and Materials Engineering Wenzhou University Guangdong Provincial key laboratory of Chemical Measurement and Emergency Test Technology (China) Institute of Analysis Guangdong Academy of Sciences (China National Analytical CenterGuangzhou)

Photocatalytic oxygen reduction for hydrogen peroxide （H2O2） synthesis presents a green and costeffective production ***,achieving highly selective H2O2synthesis remains challenging,necessitating precise control over free radical reaction pathways and minimizing undesirable oxidative ***,we report for the visible light-driven simultaneous co-photocatalytic reduction of O2to H2O2and oxidation of biomass using the atomic rubidium-nitride modified carbon nitride（CNRb）.The optimized CNRb catalyst demonstrates a record photoreduction rate of 8.01 mM h-1for H2O2generation and photooxidation rate of 3.75 mM h-1for furfuryl alcohol to furoic acid,achieving a remarkable solar-to-chemical conversion （SCC） efficiency of up to 2.27%.Experimental characterizations and DFT calculation disclosed that the introducing atomic Rb–N configurations allows for the high-selective generation of superoxide radicals while suppressing hydroxyl free radical *** is because the Rb–N serves as the new alternative site to perceive a stronger connection position for O2adsorption and reinforce the capability to extract protons,thereby triggering a high selective redox product *** study holds great potential in precisely regulating reactive radical processes at the atomic level,thereby paving the way for efficient synthesis of H2O2coupled with biomass valorization.

关键词： Atomic economy Radical pathway regulation Rubidium atom coordination biomass valorization

通过Knoevenagel缩合双酮吡咯和吲哚二噻吩得到乙烯基链接的非晶态共轭聚合物并应用于柔性晶体管（英文）

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Science China Materials 2025年第1期 110-116页

作者：陈雁琳陈品宇周仕弘杨志伟龙海军梁先峰陈天文黎静谭陆西张浩力董立春刘子桐 School of chemistry and Chemical Engineering Chongqing University State key laboratory of Applied organic chemistry (SKLAOC) Key Laboratory of Special Function Materials and Structure Design (MOE) College of Chemistry and Chemical Engineering Lanzhou University Chongqing Institute of Green and Intelligent Technology Chinese Academy of Sciences

共轭聚合物在柔性薄膜晶体管器件中展现出广泛的应用潜力.然而,设计和合成具有高迁移率与优良弯曲（或拉伸）稳定性的共轭聚合物仍面临诸多挑战.本文报道了一种具有乙烯基链接的共轭聚合物PDPPVIDT,该聚合物通过双侧甲基取代的双酮吡咯...

共轭聚合物在柔性薄膜晶体管器件中展现出广泛的应用潜力.然而,设计和合成具有高迁移率与优良弯曲（或拉伸）稳定性的共轭聚合物仍面临诸多挑战.本文报道了一种具有乙烯基链接的共轭聚合物PDPPVIDT,该聚合物通过双侧甲基取代的双酮吡咯（DPP）和茚并二噻吩（IDT）二醛单体,采用环境友好的Knoevenagel缩合反应合成.该反应条件温和,且具备良好的环境友好性及规模化潜力.研究结果表明,聚合物主链的平面性得以增强,并且显示出稳定的π-π堆积特性.此外,由于乙烯基的构象异构化特性, PDPPVIDT薄膜呈现出近乎无定形的特性,从而同时确保了电荷传输效率与柔韧性.基于PDPPVIDT的柔性有机薄膜晶体管（OTFT）器件展示出高达1.70 cm2V-1s-1的优异迁移率和良好的机械弯曲恢复能力.该研究展示了乙烯基链接D-A共轭聚合物的潜力,并强调了其生产过程的工业适应性,为未来柔性电子材料的设计与合成提供了新的思路.

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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01期 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.

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Nanostructured ZnO/BiVO_(4)I-scheme heterojunctions for piezocatalytic degradation of organic dyes via harvesting ultrasonic vibration energy

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International Journal of Minerals,Metallurgy and Materials 2025年第2期32卷 488-497页

作者： Yiling Li Xiaoyao Yu Yingjie Zhou Yao Lin Ying Wu key laboratory of the Ministry of Education for Advanced Catalysis Materials College of Chemistry and Materials ScienceZhejiang Normal UniversityJinhua 321004China

BiVO_(4)porous spheres modified by ZnO were designed and synthesized using a facile two-step *** resulting ZnO/BiVO_(4)composite catalysts have shown remarkable efficiency as piezoelectric catalysts for degrading Rhodamine B(RhB)unde mechanical vibrations,they exhibit superior activity compared to pure *** 40wt%ZnO/BiVO_(4)heterojunction composite displayed the highest activity,along with good stability and *** enhanced piezoelectric catalytic activity can be attributed to the form ation of an I-scheme heterojunction structure,which can effectively inhibit the electron-hole ***,hole(h+)and superoxide radical(·O_(2)^(-))are proved to be the primary active ***,ZnO/BiVO_(4)stands as an efficient and stable piezoelectric catalyst with broad potential application in the field of environmental water pollution treatment.

关键词： piezoelectric catalytic heterojunction dye degradation ultrasonic vibration

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Role of iron ore in enhancing gasification of iron coke:Structural evolution,influence mechanism and kinetic analysis

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International Journal of Minerals,Metallurgy and Materials 2025年第1期32卷 58-69页

作者： Jie Wang Wei Wang Xuheng Chen Junfang Bao Qiuyue Hao Heng Zheng Runsheng Xu School of chemistry and Materials Science Hubei Engineering UniversityXiaogan 432000China key laboratory for Ferrous Metallurgy and Resources Utilization of Ministry of Education Wuhan University of Science and TechnologyWuhan 430081China Institue of Ironmaking Technology Baosteel Central Research InstituteShanghai 201999China State key laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China

The utilization of iron coke provides a green pathway for low-carbon *** uncover the influence mechanism of iron ore on the behavior and kinetics of iron coke gasification,the effect of iron ore on the microstructure of iron coke was ***,a comparative study of the gasification reactions between iron coke and coke was conducted through non-isothermal thermogravimetric *** findings indicate that compared to coke,iron coke exhibits an augmentation in micropores and specific surface area,and the micropores further extend and *** provides more adsorption sites for CO_(2) molecules during the gasification process,resulting in a reduction in the initial gasification temperature of iron *** the heating rate in non-isothermal gasification can enhance the reactivity of iron *** metallic iron reduced from iron ore is embedded in the carbon matrix,reducing the orderliness of the carbon structure,which is primarily responsible for the heightened reactivity of the carbon *** kinetic study indicates that the random pore model can effectively represent the gasification process of iron coke due to its rich pore ***,as the proportion of iron ore increases,the activation energy for the carbon gasification gradually decreases,from 246.2 kJ/mol for coke to 192.5 kJ/mol for iron coke 15wt%.

关键词： low-carbon ironmaking iron coke gasification structural evolution kinetic model

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Electrocatalytic cleavage of a lignin β-O-4 model compound and coupling with nitrogen-containing aromatics using Prussian blue analogue-derived nickel–cobalt spinel

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Journal of Energy chemistry 2025年第1期100卷 628-636页

作者： Yi Qi Xueying Chen Bowen Liu Xuliang Lin Xueqing Qiu Yanlin Qin Guangdong Provincial key laboratory of Plant Resources biorefinery School of Chemical Engineering and Light Industry Guangdong University of Technology Guangdong Provincial laboratory of chemistry and Fine Chemical Engineering Jieyang Center Guangdong Basic Research Center of Excellence for Ecological Security and Green Development Guangdong University of Technology

Electrochemical conversion of lignin for the production of high-value heterocyclic aromatic compounds has great *** demonstrate the targeted synthesis and cation modulation of NiCo2O4spinel nanoboxes,synthesized via cation exchange and calcination *** catalysts exhibit excellent efficacy in the electrocatalytic conversion of lignin model compounds,specifically 2-phenoxy-1-phenylethanol,into nitrogen-containing aromatics,achieving high conversion rates and *** catalysts were synthesized via a cation exchange and calcination oxidation process,using Prussian blue nanocubes as *** porous architecture and polymetallic composition of the NiCo2O4spinel demonstrated superior performance in electrocatalytic oxidative coupling,achieving a 99.2 wt%conversion rate of the 2-phenoxy-1-phenylethanol with selectivities of 37.5 wt%for quinoline derivatives and 31.5 wt%for *** innovations include the development of a sustainable one-pot synthesis method for quinoline derivatives,the elucidation of a multistage reaction pathway involving CAO bond cleavage,hydroxyaldol condensation,and CAN bond formation,and a deeper mechanistic understanding derived from DFT *** work establishes a new strategy for lignin valorization,offering a sustainable route to produce high-value nitrogen-containing aromatics from renewable biomass under mild conditions,without the need for additional reagents.

关键词： Spinel biomass valorization Electrocatalysis Lignin oxidation Coupling

Small modifications of endo-functionalized cavities lead to large changes in molecular interaction in water

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Science China chemistry 2025年第1期 369-376页

作者： Song-Meng Wang Hao Nian Yan-Fang Wang Li-Shuo Zheng Yu-Tao Zheng Yi-Wei Dong Liping Huang Xiaoping Wang Wei Jiang Liu-Pan Yang Department of chemistry Southern University of Science and Technology School of chemistry and Pharmaceutical Sciences State Key Laboratory for Chemistry and Molecular Engineering of Medicinal ResourcesGuangxi Normal University School of Pharmaceutical Science Hengyang Medical School University of South China

Studying molecular recognition in aqueous environments is crucial for understanding biological processes. Herein, we present a series of N-doped endo-functionalized anthracene-based cavities by introducing inward-directed pyridine units. The subtle modifications can significantly affect the binding properties of these receptors, which is similar to the mutations in biological systems. Combining theoretical calculations and molecular recognition experiments demonstrated that these “mutations” have an impact on the hydrophobicity and charge distribution of the hosts, consequently significantly influencing molecular *** is crucial for understanding the intricate mechanisms of molecular-level interactions in biological receptors.

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Dative B–N bonds weaven toward two-dimensional purely organic materials for single crystals

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Science China chemistry 2025年第01期 12-14页

作者： Wei-Lei Zhou Siwei Wang Yong Chen College of chemistry and Materials Science Inner Mongolia Key Laboratory of Chemistry for Nature Products and Synthesis for Functional Molecules Innovation Team of Optical Functional Molecular Devices Inner Mongolia Minzu University College of chemistry Nankai University

Molecular topology is one of the important topics to study and understand the relationship between molecular structure and properties [1]. Particularly, two-dimensional (2D) materials with extremely high surface area and ultra-thin morphology have attracted considerable attention due to their unexpected properties in materials and chemistry [2,3].

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