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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

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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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

Electrode/Electrolyte Optimization‑Induced Double‑Layered Architecture for High‑Performance Aqueous Zinc‑(Dual)Halogen Batteries

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Nano-Micro Letters 2025年第3期17卷 121-137页

作者： Chengwang Zhou Zhezheng Ding Shengzhe Ying Hao Jiang Yan Wang Timing Fang You Zhang Bing Sun Xiao Tang Xiaomin Liu School of Textiles and Clothing School of Chemistry and Chemical EngineeringQingdao UniversityQingdao 266071ShandongPeople’s Republic of China Centre for Clean Energy Technology School of Mathematical and Physical SciencesFaculty of ScienceUniversity of Technology SydneyUltimoNSW 2007Australia School of chemistry and Chemical Engineering Henan Normal UniversityXinxiang 453007HenanPeople’s Republic of China

Aqueous zinc-halogen batteries are promising candidates for large-scale energy storage due to their abundant resources,intrinsic safety,and high theoretical ***,the uncontrollable zinc dendrite growth and spontaneous shuttle effect of active species have prohibited their practical ***,a double-layered protective film based on zinc-ethylenediamine tetramethylene phosphonic acid(ZEA)artificial film and ZnF2-rich solid electrolyte interphase(SEI)layer has been successfully fabricated on the zinc metal anode via electrode/electrolyte synergistic *** ZEA-based artificial film shows strong affinity for the ZnF2-rich SEI layer,therefore effectively suppressing the SEI breakage and facilitating the construction of double-layered protective film on the zinc metal *** double-layered architecture not only modulates Zn2+flux and suppresses the zinc dendrite growth,but also blocks the direct contact between the metal anode and electrolyte,thus mitigating the corrosion from the active *** employing optimized metal anodes and electrolytes,the as-developed zinc-(dual)halogen batteries present high areal capacity and satisfactory cycling *** work provides a new avenue for developing aqueous zinc-(dual)halogen batteries.

关键词： Zn metal anodes Double-layered protective film Electrode/electrolyte optimization Aqueous zinc-(dual)halogen batteries

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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

MoS_(2)Lubricate‑Toughened MXene/ANF Composites for Multifunctional Electromagnetic Interference Shielding

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Nano-Micro Letters 2025年第2期17卷 358-371页

作者： Jiaen Wang Wei Ming Longfu Chen Tianliang Song Moxi Yele Hao Zhang Long Yang Gegen Sarula Benliang Liang Luting Yan Guangsheng Wang School of physical Science and Engineering Beijing Jiaotong UniversityBeijing 100044People’s Republic of China Key Laboratory of Bio‑Inspired Smart Interfacial Science and Technology of Ministry of Education School of ChemistryBeihang UniversityBeijing 100191People’s Republic of China

The design and fabrication of high toughness electromagnetic interference(EMI)shielding composite films with diminished reflection are an imperative task to solve electromagnetic pollution *** MXene/ANF(aramid nanofibers)–MoS_(2)composite films with nacre-like layered structure here are fabricated after the introduction of MoS_(2)into binary MXene/ANF composite *** introduction of MoS_(2)fulfills an impressive“kill three birds with one stone”improvement effect:lubrication toughening mechanical performance,reduction in secondary reflection pollution of electromagnetic wave,and improvement in the performance of photothermal *** the introduction of MoS_(2)into binary MXene/ANF(mass ratio of 50:50),the strain to failure and tensile strength increase from 22.1±1.7%and 105.7±6.4 MPa and to 25.8±0.7%and 167.3±9.1 MPa,*** toughness elevates from 13.0±4.1 to 26.3±0.8 MJ m^(−3)(~102.3%)*** the reflection shielding effectiveness(SE_(R))of MXene/ANF(mass ratio of 50:50)decreases~10.8%.EMI shielding effectiveness(EMI SE)elevates to 41.0 dB(8.2–12.4 GHz);After the introduction of MoS_(2)into binary MXene/ANF(mass ratio of 60:40),the strain to failure increases from 18.3±1.9%to 28.1±0.7%(~53.5%),the SE_(R)decreases~22.2%,and the corresponding EMI SE is 43.9 *** MoS_(2)also leads to a more efficient photothermal conversion performance(~45 to~55℃).Additionally,MXene/ANF–MoS_(2)composite films exhibit excellent electric heating performance,quick temperature elevation(15 s),excellent cycle stability(2,2.5,and 3 V),and long-term stability(2520 s).Combining with excellent mechanical performance with high MXene content,electric heating performance,and photothermal conversion performance,EMI shielding ternary MXene/ANF–MoS_(2)composite films could be applied in many industrial *** work broadens how to achieve a balance between mechanical properties and versatility of composites in the case of high-function fillers.

关键词： MXene-MoS_(2) Lubrication toughening EMI shielding Photothermal conversion Electric heating performance

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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 Materials Chemistry and Biomedicine Innovation Center (Chem BIC) School of Chemistry and Chemical Engineering Nanjing University Green Catalysis Center College of Chemistry Zhengzhou University State Key Laboratory of Natural Medicines China Pharmaceutical University

Selective modification of peptides has always been a challenging issue. The selective alkylation of peptides can alter the biological activity and physical properties of molecules, and it has gained significant research interest. We 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 the α-C(sp3)–H in glycine residue of peptides. This 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 practicality. In 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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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68卷 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.

关键词： host-guest interaction hydrophobic effect endo-functionalized cavity mutation pyridine