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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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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

Unraveling the impacts of intermolecular interaction on morphology evolution for highly efficient organic solar cells and modules

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Science China Chemistry 2025年第1期68卷 264-272页

作者： Xueqing Ma Yingying Cheng Yuqiang Liu Xinming Zheng Guangliu Ran Hongxiang Li Xinyue Cui Andong Zhang Wenkai Zhang Pei Cheng Wenchao Huang Zhishan Bo Beijing Key Laboratory of Energy Conversion and Storage Materials College of Chemistry Beijing Normal University college of Textiles and Clothing State Key Laboratory of Bio-fibers and Eco-textiles Qingdao University Key State Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and EngineeringWuhan University of Technology Department of Physics and applied Optics Beijing Area Major Laboratory Center for Advanced Quantum Studies Beijing Normal University State Key Laboratory of Polymer Materials Engineering College of Polymer Science and Engineering Sichuan University

Understanding the effect of intermolecular interaction on the growth dynamic of active layers is critical for advancing organic solar cells(OSCs). However, the diverse structure of donors and acceptors makes the research challenging. Additives with customizable structures and properties could simplify this complexity. Herein, we meticulously tailor two additives of 3,4-ethylenedioxythiophene(EDOT) and 2,5-dibromo-3,4-ethylenedioxythiophene(DBEDOT), possessing distinct intermolecular interaction features to elaborate the inherent relationship. It is found that varied interaction strengths can alter film formation processes. The enhanced intermolecular interaction between the DBEDOT and non-fullerene acceptor BTP-e C9-4F results in pre-aggregation and longer crystallization duration of BTP-e C9-4F, facilitating the formation of films with compact molecular packing and decent phase separation. Thus, exciton dissociation and charge transport become more efficient. Finally, devices processed with DBEDOT exhibit a remarkable power conversion efficiency of 19.35% in small-area OSCs and 14.11% in bladecoated 5 cm × 5 cm organic solar mini-modules. Especially, OSCs can maintain 80% of their initial efficiency after continuous annealing at 85 °C for over 2,100 h.

关键词： organic solar cell non-fullerene acceptor film growth molecular packing intermolecular interaction

Targets capture by distributed active swarms via bio-inspired reinforcement learning

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Science China(Physics,Mechanics & Astronomy) 2025年第1期Mechanics & Astronomy) .卷 210-221页

作者： Kun Xu Yue Li Jun Sun Shuyuan Du Xinpeng Di Yuguang Yang Bo Li Institute of Biomechanics and Medical Engineering Applied Mechanics Laboratory Department of Engineering MechanicsTsinghua University Institute of Nuclear and New Energy Technology Tsinghua University Shanghai Aerospace Control Technology Institute Shanghai Key Laboratory of Aerospace Intelligent Control Technology college of Automation Engineering Nanjing University of Aeronautics and Astronautics

Natural swarms arranged from cells to herds are usually decentralized but display intriguing collective intelligence in coordinating individuals across large scales to efficiently achieve their common goals. Learning from nature may provide new strategies for controlling collective dynamics of synthetic swarms to accomplish specific functions. Here, we present a bioinspired computational framework that steers distributed active swarms to collectively capture and merge targets via reinforcement learning. We exploit collective milling structures of natural herds to cage the targets, and adopt a switching control policy inspired by sperms' chiral dynamics to optimize the trajectories of individuals, through which the active swarms can selforganize to enclose single or multiple distant targets in a dynamical, adaptive and scalable manner. There exists a critical swarm size, beyond which the excessive competition between agents would generate large mechanical forces, leading to capture instability but enabling the transition from short-distance to long-distance merging capture of multiple targets. This work provides physical insights into distributed active swarms and could offer a multilevel, decentralized strategy toward controlling swarm robotics in wide applications such as bio-medical devices, machine immunity, and target clearance.

关键词： swarm intelligence robotics multi-tasks artificial intelligence bionics

Gradient‑Layered MXene/Hollow Lignin Nanospheres Architecture Design for Flexible and Stretchable Supercapacitors

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Nano-Micro Letters 2025年第2期17卷 447-462页

作者： Haonan Zhang Cheng Hao Tongtong Fu Dian Yu Jane Howe Kaiwen Chen Ning Yan Hao Ren Huamin Zhai Jiangsu Provincial Key Lab of Sustainable Pulp and Paper Technology and Biomass Materials NanJing Forestry UniversityNanjing 210037People’s Republic of China Department of Chemical Engineering and applied Chemistry University of Toronto200 College StreetTorontoON M5S 3E5Canada Department of Materials Science and Engineering University of Toronto184 College StreetTorontoON M5S 3E4Canada college of Materials Science and Engineering Nanjing Forestry UniversityNanjing 210037People’s Republic of China

With the rapid development of flexible wearable electronics,the demand for stretchable energy storage devices has *** this work,a novel gradient-layered architecture was design based on single-pore hollow lignin nanospheres(HLNPs)-intercalated two-dimensional transition metal carbide(Ti_(3)C_(2)T_(x) MXene)for fabricating highly stretchable and durable *** depositing and inserting HLNPs in the MXene layers with a bottom-up decreasing gradient,a multilayered porous MXene structure with smooth ion channels was constructed by reducing the overstacking of MXene ***,the micro-chamber architecture of thin-walled lignin nanospheres effectively extended the contact area between lignin and MXene to improve ion and electron accessibility,thus better utilizing the pseudocapacitive property of *** these strategies effectively enhanced the capacitive performance of the *** addition,HLNPs,which acted as a protective phase for MXene layer,enhanced mechanical properties of the wrinkled stretchable electrodes by releasing stress through slip and deformation during the stretch-release cycling and greatly improved the structural integrity and capacitive stability of the *** electrodes and symmetric flexible all-solid-state supercapacitors capable of enduring 600%uniaxial tensile strain were developed with high specific capacitances of 1273 mF cm^(−2)(241 F g^(−1))and 514 mF cm^(−2)(95 F g^(−1)),***,their capacitances were well preserved after 1000 times of 600%stretch-release *** study showcased new possibilities of incorporating biobased lignin nanospheres in energy storage devices to fabricate stretchable devices leveraging synergies among various two-dimensional nanomaterials.

关键词： Hollow lignin nanospheres MXene Gradient-layered architecture Wrinkled electrodes Stretchable supercapacitors

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Congruent Feature Selection Method to Improve the Efficacy of Machine Learning-Based Classification in Medical Image Processing

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Computer Modeling in Engineering & Sciences 2025年第1期142卷 357-384页

作者： Mohd Anjum Naoufel Kraiem Hong Min Ashit Kumar Dutta Yousef Ibrahim Daradkeh Department of Computer Engineering Aligarh Muslim UniversityAligarh202002India college of Computer Science King Khalid UniversityAbha61413Saudi Arabia School of Computing Gachon UniversitySeongnam13120Republic of Korea Department of Computer Science and Information Systems College of Applied SciencesAlMaarefa UniversityRiyadh13713Saudi Arabia Department of Computer Engineering and Information College of Engineering in Wadi AlddawasirPrince Sattam bin Abdulaziz UniversityAl-Kharj16273Saudi Arabia

Machine learning(ML)is increasingly applied for medical image processing with appropriate learning *** applications include analyzing images of various organs,such as the brain,lung,eye,etc.,to identify specific flaws/diseases for *** primary concern of ML applications is the precise selection of flexible image features for pattern detection and region *** of the extracted image features are irrelevant and lead to an increase in computation ***,this article uses an analytical learning paradigm to design a Congruent Feature Selection Method to select the most relevant image *** process trains the learning paradigm using similarity and correlation-based features over different textural intensities and pixel *** similarity between the pixels over the various distribution patterns with high indexes is recommended for disease ***,the correlation based on intensity and distribution is analyzed to improve the feature selection ***,the more congruent pixels are sorted in the descending order of the selection,which identifies better regions than the ***,the learning paradigm is trained using intensity and region-based similarity to maximize the chances of ***,the probability of feature selection,regardless of the textures and medical image patterns,is *** process enhances the performance of ML applications for different medical image *** proposed method improves the accuracy,precision,and training rate by 13.19%,10.69%,and 11.06%,respectively,compared to other models for the selected *** mean error and selection time is also reduced by 12.56%and 13.56%,respectively,compared to the same models and dataset.

关键词： Computer vision feature selection machine learning region detection texture analysis image classification medical images

Multi boron-doping effects in hard carbon toward enhanced sodium ion storage

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Journal of Energy Chemistry 2025年第1期100卷 730-738页

作者： Peng Zheng Wang Zhou Ying Mo Biao Zheng Miaomiao Han Qin Zhong Wenwen Yang Peng Gao Lezhi Yang Jilei Liu college of Materials Science and Engineering Hunan Joint International Laboratory of Advanced Materials and Technology for Clean Energy Hunan Province Key Laboratory for Advanced Carbon Materials and Applied Technology Hunan University Greater Bay Area Institute for Innovation Hunan University Changsha Research Institute of Mining & Metallurgy Co. LTD.

Hard carbon （HC） has been considered as promising anode material for sodium-ion batteries （SIBs）.The optimization of hard carbon’s microstructure and solid electrolyte interface （SEI） property are demonstrated effective in enhancing the Na+storage capability,however,a one-step regulation strategy to achieve simultaneous multi-scale structures optimization is highly ***,we have systematically investigated the effects of boron doping on hard carbon’s microstructure and interface chemistry.A variety of structure characterizations show that appropriate amount of boron doping can increase the size of closed pores via rearrangement of carbon layers with improved graphitization degree,which provides more Na+storage ***-situ Fourier transform infrared spectroscopy/electrochemical impedance spectroscopy （FTIR/EIS） and X-ray photoelectron spectroscopy （XPS） analysis demonstrate the presence of more BC3and less B–C–O structures that result in enhanced ion diffusion kinetics and the formation of inorganic rich and robust SEI,which leads to facilitated charge transfer and excellent rate *** a result,the hard carbon anode with optimized boron doping content exhibits enhanced rate and cycling *** general,this work unravels the critical role of boron doping in optimizing the pore structure,interface chemistry and diffusion kinetics of hard carbon,which enables rational design of sodium-ion battery anode with enhanced Na+storage performance.

关键词： X ray photoelectron spectroscopy