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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 {1. 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-1.nd long-term durability (over1.70 h at 1. m A cm-2and 1.0 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

Ultrastrong room-temperature phosphorescence in cucurbit[8]uril-mediated crystalline supramolecules for ratiometric detection of phenethylamine

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Science China chemistry 2025年

作者： Qingyu Niu Yingxiang Ye Lingna Su Xu He Zhiqiang Li Yu Liu School of Chemical Engineering and Technology Hebei University of Technology Fujian Provincial key {1. of Polymer Materials College of Chemistry and Materials Science Fujian Normal University key {1. of Advanced Energy Materials chemistry (Ministry of Education) Nankai University College of chemistry State Key Laboratory of Elemento-Organic Chemistry Nankai University

It is a great challenge to modulate purely organic fluorescence-phosphorescence dual emission in aqueous solution because the excited singlet and triplet {1.s are in competition with each other. Herein, we report a crystalline 1.2 host-guest formed by selfassembly of 4-(4-bromophenyl)-pyridinium derivatives and cucurbit[8]uril, in which a rigid environment rich in weak interactions is directly demonstrated. Due to the inhibition of non-radiative transition and stabilization of triplet exciton in the crystalline environment, the crystalline inclusion complex exhibits ultralong room-temperature phosphorescence lifetime of 3.21.ms with an room-temperature phosphorescence(RTP) quantum yield up to 1..29%. Interestingly, the crystalline 1.2 hostguest complex demonstrates the ability of rapid identification and sensitive fluorescence-phosphorescence ratiometric detection behavior toward phenethylamine, a drug analogue, with a limit of detection as low as 27.5 nM. We believe that this study will undoubtedly broaden the utilizing scopes of RTP and offer a novel avenue for psychoactive substances monitoring.

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Boosting hydrocarbon conversion via Cu-doping induced oxygen vacancies on CeO2 in CO2 electroreduction

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Journal of Energy chemistry 2025年第1期100卷 66-76页

作者： Lei Xue Tong Shi Chenhui Han Heng Zhang Fenrong Liu Haorun Li Yan Wang Xiaojun Gu Shanghong Zeng Inner Mongolia key {1. of chemistry and Physics of Rare Earth Materials School of Chemistry and Chemical Engineering Inner Mongolia University state {1. laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences institute of Catalysis Department of Chemistry Zhejiang University National key {1. of Baiyunobo Rare Earth Resource Research and Comprehensive Utilization Baotou Research Institute of Rare Earths

Conversion of CO2back to hydrocarbons is the most direct way of closing the“carbon cycle”,and its significance is further enlarged if this process is driven by renewable energies such as ***,precisely controlling the product selectivity towards hydrocarbons against the competitive hydrogen evolution remains challenging,especially for Cu-based ***,we report a novel defect engineering strategy,by which Cu-doping-induced oxygen vacancies on CeO2nanorods were effectively created,with adjustable vacancy/Cu *** resulting optimum catalyst shows up to 79% catalytic current density to hydrocarbons （excluding CO）,with 49% faradaic efficiency to *** and density functional theory unveil that the ratio between oxygen vacancy and Cu affects significantly the formation of*CHO and activation of H2O,which leads to the following deep hydrogenation to *** findings may spur new insights for designing and developing more controllable chemical process relevant to CO2utilization.

关键词： Nanorods

Photosynthetic reaction pathways of natural and artificial systems

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Science China chemistry 2025年

作者： Shixing Lei Liting Bi Lingxuan Chen Zhanting Li Jia Tian state {1. laboratory of Organometallic chemistry and Shanghai Hong Kong Joint laboratory in Chemical Synthesis Shanghai Institute of Organic Chemistry University of Chinese Academy of Sciences Chinese Academy of Sciences

Photosynthesis converts solar energy into chemical energy through highly coordinated photosynthetic *** by natural systems,artificial photosynthesis aims to develop an efficient,sustainable,and cost-effective pathway for solar-tochemical *** review examines natural photosynthetic pathways,including retinal/rhodopsin-,bacteriochlorophyll-,and chlorophyll-based systems,highlighting their key components and ***,we outline reaction pathways in artificial photosynthetic systems constructed via heterogeneous,homogeneous,self-assembly,and semi-artificial strategies,focusing on water splitting,carbon fixation,and nitrogen ***,we offer insights into future directions for artificial photosynthesis,emphasizing the importance of using self-assembly strategies and the potential of using primitive phototrophic microorganisms as models.

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Enhanced subacute ischemic stroke treatment via multistage drug delivery system design for combination therapy

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Science China chemistry 2025年

作者： Xihan Xu Juan-Juan Li Jiamin Li Hui-Yan Zhang Yilin Qi Bing-Sen Shi Tianqi Li Shan-Shan Su Weitao Zhao Chang Chen Zhongying Gong Huiyu Liu Ke-Rang Wang Dong-Sheng Guo Xue Xue state {1. laboratory of Medicinal Chemical Biology College of Pharmacy Nankai University College of chemistry State Key Laboratory of Elemento-Organic Chemistry Key Laboratory of Functional Polymer Materials (Ministry of Education) Frontiers Science Center for New Organic Matter Collaborative Innovation Center of Chemical Science and EngineeringNankai University College of chemistry and Materials Science State Key Laboratory of New Pharmaceutical Preparations and Excipients Key Laboratory of Medicinal Chemistry and Molecular Diagnosis (Ministry of Education) Key Laboratory of Chemical Biology of Hebei Province Hebei Research Center of the Basic Discipline of Synthetic Chemistry Hebei University Department of Neurology Tianjin First Central Hospital School of Medicine Nankai University Beijing Advanced Innovation Center for Soft Matter Science and Engineering State Key Laboratory of Organic-Inorganic Composites Beijing Laboratory of Biomedical Materials Bionanomaterials & Translational Engineering Laboratory Beijing Key Laboratory of BioprocessBeijing University of Chemical Technology

The management of acute ischemic stroke remains challenging due to its abrupt onset and the narrow treatment window,resulting in high rates of disability and *** therapy for neuroprotection and neurorepair strategies provided new hopes for subacute stroke *** we designed a multistage nanodelivery system that matches the unique microenvironment of the subacute phase of stroke,which utilizes calixarene as a building block to effectively load the neuroprotective drug *** calixarene is designed with glycosidic linkages targeting the glucose transporter 1.(GLUT1.on the blood-brain barrier (BBB) and azo bonds that are responsive to hypoxic ***,the decomposed calixarene molecules themselves possess intrinsic bio-activation to modulate inflammatory responses,achieving a multistage therapeutic approach that transitions from targeting to release and finally to *** approach combines anti-inflammation and neuroprotection,providing a multi-level treatment *** system was validated in a rat model of permanent middle cerebral artery occlusion (pMCAO),demonstrating that intravenous administration of the nanodelivery system repairs brain damage and improves motor function 24 h post-pMCAO *** work offers a precise and integrative strategy for stroke patients missing the acute therapy window to improve functional recovery and enhance the effect of comprehensive treatment.

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An Unprecedented Efficiency with Approaching 21.Enabled by Additive‑Assisted Layer‑by‑Layer Processing in organic Solar Cells

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Nano-Micro Letters 2025年第2期17卷 372-375页

作者： Shuai Xu Youdi Zhang Yanna Sun Pei Cheng Zhaoyang Yao Ning Li Long Ye Lijian Zuo Ke Gao key {1. of Advanced Green Functional Materials College of ChemistryChangchun Normal UniversityChangchun 130032People’s Republic of China Shandong Provincial key {1. for Science of Material Creation and Energy Conversion School of Chemistry and Chemical EngineeringShandong UniversityQingdao 266237People’s Republic of China College of Polymer Science and Engineering Sichuan UniversityChengdu 610065People’s Republic of China state {1. laboratory and institute of elemento‑organic chemistry Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer MaterialsRenewable Energy Conversion and Storage Center(RECAST)College of ChemistryNankai UniversityTianjin 300071People’s Republic of China institute of Polymer Optoelectronic Materials and Devices {1. key laboratory of Luminescent Materials and Devices South China University of TechnologyGuangzhou 510640People’s Republic of China Tianjin key {1. of Molecular Optoelectronic Sciences School of Materials Science and EngineeringTianjin UniversityTianjin 300350People’s Republic of China state {1. laboratory of Silicon Materials MOE Key Laboratory of Macromolecular Synthesis and FunctionalizationDepartment of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China

Recently published in Joule,Feng Liu and colleagues from Shanghai Jiaotong University reported a record-breaking 20.8%power conversion efficiency in organic solar cells(OSCs)with an interpenetrating fibril network active layer morphology,featuring a bulk p-in structure and proper vertical segregation achieved through additive-assisted layer-by-layer *** optimized hierarchical gradient fibrillar morphology and optical management synergistically facilitates exciton diffusion,reduces recombination losses,and enhances light capture *** approach not only offers a solution to achieving high-efficiency devices but also demonstrates the potential for commercial applications of OSCs.

关键词： organic solar cells Additive-assisted layer-by-layer processing Three-dimensional fibril morphology Bulk p-i-n structure Optical management

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Photoinduced radical sulfur dioxide insertion with asymmetric cyclization of alkenes: accessing β-chiral sulfones bearing S-stereocentric cyclic sulfinamides

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Science China chemistry 2025年第01期 257-263页

作者： Jiapian Huang Chenxin Wang Xu Wang Xiaoyu Zhou Wei Xiao Jie Wu School of Pharmaceutical and Chemical Engineering & institute for Advanced Studies Taizhou University state {1. laboratory of Organometallic chemistry Shanghai Institute of Organic Chemistry Chinese Academy of Sciences School of chemistry and Chemical Engineering Henan Normal University

The generation of various β-chiral sulfones bearing chiral cyclic sulfinamides through photoredox-catalyzed sulfur dioxide insertion with asymmetric radical cyclization is described. This method features a broad substrate scope and excellent stereospecificity. Computational studies reveal that the dispersion interaction between sulfinyl group and CH2SO2Ph group plays a crucial role in the stereoselectivity control.

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Low-cost and fluoride-free synthesis of MFI zeolite nanosheets with enhanced stability for benzene alkylation with ethanol

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Journal of Energy chemistry 2025年第1期100卷 458-468页

作者： Peng Zhu Cun Liu Yiren Yu Guoshu Gao Yumeng Zhao Xiongfu Zhang Guodong Liu Guohui Yang state {1. laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology state {1. laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences

Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive structure-directing agents(SDAs), pricey raw materials, and eco-unfriendly fluorine-containing additives. Here, we contributed a cost-effective and fluoride-free synthesis method for synthesizing high-quality MFI zeolite nanosheets through a Silicalite-1.Sil-1. seed suspension and urea cooperative strategy, only with inexpensive colloidal silica as the Si source. Our approach was effective for synthesizing both Sil-1.and aluminum-containing ZSM-5 nanosheets. By optimizing key synthesis parameters,including seed aging time, seed quantity, and urea concentration, we achieved precise control over the crystal face aspect ratio and b-axis thickness. We also revealed a non-classical oriented nanosheet growth mechanism, where Sil-1.seeds induced the formation of quasi-ordered precursor particles, and the(01.)crystal planes of these particles facilitated urea adsorption, thereby promoting c-axis-oriented *** obtained ZSM-5 nanosheets exhibited exceptional catalytic performance in the benzene alkylation with ethanol, maintaining stability for over 500 h, which is 5 times longer than traditional ZSM-5 catalysts. Furthermore, large-scale production of ZSM-5 nanosheets was successfully carried out in a 3 L highpressure autoclave, yielding samples consistent with those from {1.-scale synthesis. This work marks a significant step forward in the sustainable and efficient production of MFI nanosheets using inexpensive and environmentally friendly raw materials, offering the broad applicability in catalysis.

关键词： Aspect ratio

Deciphering Water Oxidation Catalysts:The Dominant Role of Surface chemistry over Reconstruction Degree in Activity Promotion

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Nano-Micro Letters 2025年第3期17卷 340-354页

作者： Li An Jianyi Li Yuanmiao Sun Jiamin Zhu Justin Zhu Yeow Seow Hong Zhang Nan Zhang Pinxian Xi * Zhichuan JXu Chun‑Hua Yan state {1. laboratory of Applied organic chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu ProvinceFrontiers Science Center for Rare IsotopesCollege of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000People’s Republic of China School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798Singapore Faculty of Materials Science and Energy Engineering Institute of Technology for Carbon NeutralityShenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055People’s Republic of China key {1. of Electromagnetic Materials and Devices National Center for International Research On Photoelectric and Energy MaterialsSchool of Materials and EnergyElectron Microscopy CenterYunnan UniversityKunming 650091People’s Republic of China state {1. laboratory of Baiyunobo Rare Earth Resource Researches and Comprehensive Utilization Baotou Research Institute of Rare EarthsBaotou 014030People’s Republic of China Beijing National laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU‑HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryPeking UniversityBeijing 100871People’s Republic of China

Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution *** surface reconstruction has been widely observed in perovskite catalysts,and the reconstruction degree has been often correlated with the activity ***,a systematic study on the roles of Fe substitution in activation of perovskite LaNiO_(3)is *** substituting Fe content influences both current change tendency and surface reconstruction ***_(0.9)Fe_(0.1.O_(3)is found exhibiting a volcano-peak intrinsic activity in both pristine and reconstructed among all substituted perovskites in the LaNi_(1.x)Fe_(x)O_(3)(x=0.00,0.1.,0.25,0.50,0.75,1.00)*** reconstructed LaNi_(0.9)Fe_(0.1.O_(3)shows a higher intrinsic activity than most reported NiFe-based ***,density functional theory calculations reveal that Fe substitution can lower the O 2p level,which thus stabilize lattice oxygen in LaNi0.9Fe0.1.3 and ensure its long-term ***,it is vital interesting that activity of the reconstructed catalysts relied more on the surface chemistry rather than the reconstruction *** effect of Fe on the degree of surface reconstruction of the perovskite is decoupled from that on its activity enhancement after surface *** finding showcases the importance to customize the surface chemistry of reconstructed catalysts for water oxidation.

关键词： Oxygen evolution reaction Perovskite oxides Doping Activation and reconstruction