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Insights into ionic association boosting water oxidation activity and dynamic stability

Journal of Energy Chemistry 2024年第2期89卷 99-109,I0004页

作者： Zanling Huang Shuqi Zhu Yuan Duan Chaoran Pi Xuming Zhang Abebe Reda Woldu jing-xin jian Paul K.Chu Qing-Xiao Tong Liangsheng Hu Xiangdong Yao Department of Chemistry and Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province Shantou UniversityShantou 515063GuangdongChina Chemistry and Chemical Engineering Guangdong Laboratory Shantou 515063GuangdongChina State Key Laboratory of Refractories and Metallurgy and Institute of Advanced Materials and Nanotechnology Wuhan University of Science and TechnologyWuhan 430081HubeiChina Department of Physics Department of Materials Science and Engineeringand Department of Biomedical EngineeringCity University of Hong KongTat Chee AvenueKowloonHong KongChina School of Advanced Energy Sun Yat-sen University(Shenzhen)Shenzhen 518107GuangdongChina

There have been reports about Fe ions boosting oxygen evolution reaction(OER)activity of Ni-based catalysts in alkaline conditions,while the origin and reason for the enhancement remains ***,we attempt to identify the activity improvement and discover that Ni sites act as a host to attract Fe(Ⅲ)to form Fe(Ni)(Ⅲ)binary centres,which serve as the dynamic sites to promote OER activity and stability by cyclical formation of intermediates(Fe(Ⅲ)→Fe(Ni)(Ⅲ)→Fe(Ni)-OH→Fe(Ni)-O→Fe(Ni)OOH→Fe(Ⅲ))at the electrode/electrolyte interface to emit O_(2).Additionally,some ions(Co(Ⅱ),Ni(Ⅱ),and Cr(Ⅲ))can also be the active sites to catalyze the OER process on a variety of *** Fe(Ⅲ)-catalyzed overall water-splitting electrolyzer comprising bare Ni foam as the anode and Pt/Ni-Mo as the cathode demonstrates robust stability for 1600 h at 1000 mA cm^(-2)@~1.75 *** results provide insights into the ioncatalyzed effects boosting OER performance.

关键词： Oxygen evolution reaction Fe(Ⅲ)-catalysis Ni-Fe binary active centers Ion-catalyzed effects Robust stability

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Dangling Ligand Enables an Iron Hexa-Coordinated Molecular Catalyst for Water Oxidation by Photocatalysis

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CCS Chemistry 2024年第3期6卷 623-630页

作者： Bing Yang Qi Liu Xiang-Zhu Wei Tao Lei Qing-Qing Yang Xu-Zhe Wang jing-xin jian xin jiang Chen-Ho Tung Li-Zhu Wu Key Laboratory of Photochemical Conversion and Optoelectronic Materials New Cornerstone Science LaboratoryTechnical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190 School of Future Technology University of Chinese Academy of SciencesBeijing 100049

Photocatalytic water oxidation reaction by transition metal complexes remains a challenge because of their poor stability under irradiation,especially for earth-abundant metal *** this regard,ironbased water oxidation catalysts are prone to hydrolysis and/or dissociate the ligands to form nanoparticles under a real catalytic ***,we describe a unique hexa-coordinated catalyst 1[Fe^(II)(Py_(3)tacn)Cl_(2)]and its reference 2[Fe^(II)(PhPy_(2)tacn)Cl_(2)]with a dangling pyridyl ligand and a phenyl group,*** anticipated that the dynamically open and close coordination behaviors of the pyridyl ligand enabled balance of the reactivity and stability of catalyst *** our delight,the“open form”of catalyst 1 provided a free coordination site,and the“close form”guaranteed its molecular integrity,resulting in a water oxidation reaction with high efficiency and *** turnover number and turnover frequency values of 2332 and 60 s^(−1)are the highest known to date among iron-based homogeneous water oxidation systems under visible light irradiation.

关键词： water oxidation photocatalysis homogeneous catalysis iron complexes dangling ligand intermediates characterization

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Two paths, one goal: mechanism of calcium homeostasis to balance plant growth and immunity

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Science China Life Sciences 2025年第1期68卷 306-308页

作者： Aziz Ul Ikram Yanping jing Huan Chen jian Chen International Genome Center Jiangsu University Joint Center for Single Cell Biology School of Agriculture and BiologyShanghai Jiao Tong University

Calcium(Ca2+) is an essential nutrient and a cellular signal in plants. The level of free Ca2+in the apoplast is ～10,000-fold higher than that in the cytoplasm at the resting state. This large Ca2+level gradient across the membrane between the interior and exterior can cause Ca2+overload and toxicity. Plants have evolved mechanisms to export Ca2+out of the cytoplasm or store it in intracellular organelles, such as endoplasmic reticulum（ER）, mitochondria, and vacuole.

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High-throughput screening of CO_(2) cycloaddition MOF catalyst with an explainable machine learning model

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Green Energy & Environment 2025年第1期10卷 132-138页

作者： Xuefeng Bai Yi Li Yabo Xie Qiancheng Chen xin Zhang jian-Rong Li Beijing Key Laboratory for Green Catalysis and Separation and Department of Chemical Engineering College of Materials Science&EngineeringBeijing University of TechnologyBeijing100124China

The high porosity and tunable chemical functionality of metal-organic frameworks(MOFs)make it a promising catalyst design ***-throughput screening of catalytic performance is feasible since the large MOF structure database is *** this study,we report a machine learning model for high-throughput screening of MOF catalysts for the CO_(2) cycloaddition *** descriptors for model training were judiciously chosen according to the reaction mechanism,which leads to high accuracy up to 97%for the 75%quantile of the training set as the classification *** feature contribution was further evaluated with SHAP and PDP analysis to provide a certain physical understanding.12,415 hypothetical MOF structures and 100 reported MOFs were evaluated under 100℃ and 1 bar within one day using the model,and 239 potentially efficient catalysts were *** them,MOF-76(Y)achieved the top performance experimentally among reported MOFs,in good agreement with the prediction.

关键词： Metal-organic frameworks High-throughput screening Machine learning Explainable model CO_(2)cycloaddition

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Structural designs and mechanism insights into electrocatalytic oxidation of 5-hydroxymethylfurfural

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Journal of Energy Chemistry 2025年第1期100卷 792-814页

作者： jing Lei Huijie Zhang jian Yang Jia Ran Jiqiang Ning Haiyan Wang Yong Hu Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Department of Chemistry Zhejiang Normal University Jinhua Advanced Research Institute Department of Optical Science and Engineering Fudan University College of Chemistry and Materials Engineering Zhejiang A&F University

Biomass conversion offers an efficient approach to alleviate the energy and environmental *** oxidation of 5-hydroxymethylfurfural(HMF) has attracted tremendous attention in the latest few years for the mild synthesis conditions and high conversion efficiency to obtain 2,5-furan dicarboxylic acid(FDCA), but there still remain problems such as limited yield, short cycle life,and ambiguous reaction mechanism. Despite many reviews highlighting a variety of electrocatalysts for electrochemical oxidation of HMF, a detailed discussion of the structural modulation of catalyst and the underlying catalytic mechanism is still lacking. We herein provide a comprehensive summary of the recent development of electrochemical oxidation of HMF to FDCA, particularly focusing on the mechanism studies as well as the advanced strategies developed to regulate the structure and optimize the performance of the electrocatalysts, including heterointerface construction, defect engineering,single-atom engineering, and in situ reconstruction. Experimental characterization techniques and theoretical calculation methods for mechanism and active site studies are elaborated, and challenges and future directions of electrochemical oxidation of HMF are also prospected. This review will provide guidance for designing advanced catalysts and deepening the understanding of the reaction mechanism beneath electrochemical oxidation of HMF to FDCA.

关键词： Structural design

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Dielectric-ion-conductive ZnNb2O6 layer enabling rapid desolvation and diffusion for dendrite-free Zn metal batteries

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Journal of Energy Chemistry 2025年第1期100卷 693-701页

作者： Haifeng Yang jian Wang Panpan Zhang Xiaomin Cheng Qinghua Guan jing Dong Bixian Chen Lujie Jia jing Zhang Yongzheng Zhang Yunjian Liu Hongzhen Lin School of Materials Science and Engineering Jiangsu University i-Lab & CAS Key Laboratory of Nanophotonic Materials and Devices Suzhou Institute of Nano-Tech and Nano-Bionics Chinese Academy of Sciences Helmholtz Institute Ulm (HIU) Karlsruhe Institute of Technology (KIT) School of Materials Science and Engineering Xi'an University of Technology State Key Laboratory of Chemical Engineering East China University of Science and Technology

Rechargeable aqueous zinc-metal batteries （AZMBs） are promising candidates for large-scale energy storage systems due to their low cost and high ***,their performance and sustainability are significantly hindered by the sluggish desolvation kinetics at the electrode/electrolyte interface and the corresponding hydrogen evolution reaction where active water molecules tightly participate in the Zn（H2O）62+solvation ***,learnt from self-generated solid electrolyte interphase （SEI） in anodes,the dielectric but ion-conductive zinc niobate nanoparticles artificial layer is constructed on metallic Zn surface （ZNB@Zn）,acting as a rapid desolvation *** zincophilic and dielectric-conductive properties of ZNB layer accelerate interfacial desolvation/diffusion and suppress surface corrosion or dendrite formation,achieving uniform Zn plating/stripping behavior,as confirmed by electronic/optical microscopies and interface spectroscopical measurements together with theoretical ***,the as-prepared ZNB@Zn electrode exhibits excellent cycling stability of over 2000 h and robust reversibility （99.54%） even under high current density and depth of discharge ***,the assembled ZNB@Zn-based full cell displays high capacity-retention rate of 80.21%after 3000 cycles at 5 A g-1and outstanding rate performance up to 10 A *** large-areal pouch cell is stabilized for hundreds of cycles,highlighting the bright prospects of the dielectric but ion-conductive layer in further application of AZMBs.

关键词： Zn metal battery Dielectric artificial layer Rapid ion diffusion Zincophilic diffusion Active water inhibition

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Comparative proteomic analysis of plasma exosomes reveals the functional contribution of N-acetyl-alpha-glucosaminidase to Parkinson’s disease

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Neural Regeneration Research 2025年第10期20卷 2998-3012页

作者： Yuan Zhao Yidan Zhang xin Liu jian Zhang Ya Gao Shuyue Li Cui Chang Xiang Liu Guofeng Yang Department of Geriatrics Second Hospital of Hebei Medical UniversityShijiazhuangHebei ProvinceChina Department of Neurosurgery The Second Hospital of Hebei Medical UniversityShijiazhuangHebei ProvinceChina

Parkinson’s disease is the second most common progressive neurodegenerative disorder,and few reliable biomarkers are available to track disease *** proteins,DNA,mRNA,and lipids carried by exosomes reflect intracellular changes,and thus can serve as biomarkers for a variety of *** this study,we investigated alterations in the protein content of plasma exosomes derived from patients with Parkinson’s disease and the potential therapeutic roles of these proteins in Parkinson’s *** a tandem mass tag-based quantitative proteomics approach,we characterized the proteomes of plasma exosomes derived from individual patients,identified exosomal protein signatures specific to patients with Parkinson’s disease,and identified N-acetyl-alpha-glucosaminidase as a differentially expressed protein.N-acetyl-alpha-glucosaminidase expression levels in exosomes from the plasma of patients and healthy controls were validated by enzyme-linked immunosorbent assay and western *** results demonstrated that the exosomal N-acetyl-alpha-glucosaminidase concentration was not only lower in Parkinson’s disease,but also decreased with increasing Hoehn-Yahr stage,suggesting that N-acetyl-alpha-glucosaminidase could be used to rapidly evaluate Parkinson’s disease ***,western blot and immunohistochemistry analysis showed that N-acetyl-alpha-glucosaminidase levels were markedly reduced both in cells treated with 1-methyl-4-phenylpyridinium and cells overexpressingα-synuclein compared with control ***,N-acetyl-alpha-glucosaminidase overexpression significantly increased cell viability and inhibitedα-synuclein expression in 1-methyl-4-phenylpyridinium-treated *** together,our findings demonstrate for the first time that exosomal N-acetyl-alpha-glucosaminidase may serve as a biomarker for Parkinson’s disease diagnosis,and that N-acetyl-alpha-glucosaminidase may reduceα-synuclein expression and 1-methyl-4-phenylpyridinium-induced n

关键词： biomarker diagnosis exosomes N-acetyl-alpha-glucosaminidase Parkinson’s disease proteomic α-synuclein

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纤维级聚酯切片色相测试方法讨论

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聚酯工业 2019年第2期32卷 11-15页

作者：景新建中石化股份有限公司天津分公司化验计量中心天津300270

色相是纤维级聚酯切片的一项重要指标,它最直观地反应切片的品质,在实际生产中,能够及时快速、准确测定聚酯切片色相,对指导聚酯装置生产有着重要意义。国标中,纤维级聚酯切片色相的分析包括"干燥粉碎法"及"切粒法"2种方法,通过对比2种... 详细信息

色相是纤维级聚酯切片的一项重要指标,它最直观地反应切片的品质,在实际生产中,能够及时快速、准确测定聚酯切片色相,对指导聚酯装置生产有着重要意义。国标中,纤维级聚酯切片色相的分析包括"干燥粉碎法"及"切粒法"2种方法,通过对比2种色相测试方法,"切粒法"更为简单、快速,能够及时指导聚酯装置切片生产调整。可以在生产中改用"切粒法"测试聚酯切片色度,改用"切粒法"后,与之前"干燥粉碎法"色度差值ΔL平均值为7.87,Δb值平均值为1.91。

关键词：聚酯切片纤维级色相测试方法对比

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Identification and Characterization of Two Putative SAC Genes Involved in Fungal Development and Benzimidazole Resistance in Gibberella zeae

Identification and Characterization of Two Putative SAC Gene...

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中国植物病理学会2012年学术年会

作者： ZHANG Lei-Gang YU xin-Yan JIA Xiao-jing WANG jian-xin CHEN Chang-Jun ZHOU Ming-Guo~* (College of Plant Protection,Nanjing Agricultural University,Nanjing,China)

Resistance to carbendazim and other benzimidazole fungicides in Gibberella zeae is conferred by point mutations in theβ-tubulin gene,a gene that plays an important role in spindle assembly. The spindle assembly checkpoint is a cellular surveillance system that ensures the fidelity of chromosome segregation,which is critical for maintaining genomic *** this study,we isolated and characterized two predicted checkpoint protein-encoding genes(Mad2 and Bub1 ) in *** and designated them as FgMad2 and FgBub1,*** sequenced the two genes in two parental strains(one was sensitive to carbendazim while the other was highly resistant) and found no mutation,indicating that the resistance did not result from mutation of the two checkpoint *** FgMad2 deletion mutants grew slowlier and produced fewer conidia,both hyphae and conidia ***,the deletion of FgBub1 had no effect on fungal development other than a 47.7%～48.2%reduction in conidia ***2 deletion mutants exhibited a severe decrease(from 89.6%-90.4%) in perithecia production and pathogenicity along with a 39.5%～47.2%down-regulation of deoxynivalenol synthesis, whereas FgBub1 deletion mutants exhibited only a slight reduction in perithecia production but their pathogenicity was decreased by 51.1%～54.8%;these results suggested that asexual development,sexual development,and pathogenicity depend more on FgMad2 than on ***,the decrease in the pathogenicity of FgBub1 deletion mutants was accompanied by a two-fold increase in deoxynivalenol *** sensitivity of FgMad2 and FgBub1 deletion mutants to benzimidazole fungicides were both enhanced,especially for mutants original from MBC-high-resistant strain ***,parental strains and theirβ orβ -tubulin deletion mutants displayed high Mad2 expression when treated with MBC,which was not observed for Bub1,suggesting that FgMad2 responsed to spindle damage resulted from *** can

关键词： Gibberella zeae spindle assembly checkpoint Mad2 Bub1 benzimidazole resistance

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Breaking the structural symmetry of active sites in zeolite imidazolate framework for enhanced CO2 photoreduction

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Science China Chemistry 2025年

作者： Yupeng Han Yayu Yan Qiaohong Li xin Wu Fei Wang jian Zhang State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences University of Chinese Academy of Sciences College of Chemistry Fuzhou University

Adjusting the structure and composition of active sites is a highly effective method for activating linear ***, precise control of interfacial chemistry within molecular-scale environments presents a significant challenge in heterogeneous catalysis. In our study, we present symmetry-broken Mo-O-Co triple-atom active sites within the hybrid zeolite imidazole framework HZIF-CoMo. These sites disrupt the electronic balance and create a weak built-in electric field, thus promoting photocatalytic CO2reduction. The CO yield over HZIF-CoMo is improved to 3.1 mmol g-1h-1, which is over four times higher than the parent cobalt-imidazole framework MAF-6-Co. Both experimental and theoretical studies indicate that electronic modulation through the symmetry-breaking Mo-O-Co moiety acts as an organizing knob to accelerate charge separation and result in more carriers participating in the catalytic reaction. This work provides important insights into optimizing site-related electronic structures for targeted photocatalytic reactions.

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