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Chinese Journal of Chemistry 2024年第7期42卷 705-710页

作者： juan Wang Qing-Xian Xie Xiang Li Chang-Bin Yu Yong-Gui Zhou School of Chemistry Dalian University of Technology2 Linggong RoadDalianLiaoning 116024China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianLiaoning 116023China

The planar-chiral ligands have been widely applied as a class of unique and significant ligands in asymmetric catalysis.Among them,chiral[2.2]paracycyclophane has emerged as a privileged type of planar-chiral framework and has been utilized as an important toolbox due to their structural stability.Herein,we design and synthesize[2.2]paracyclophane-derived oxazole-pyrimidine ligands(abberviated as PYMCOX).These N,N-ligands with stable properties,rigid structure and large steric hindrance performed successfully in nickel-catalyzed asymmetric 1,2-reduction ofα,β-unsaturated ketones,affording the chiral allylic alcohols with up to 99%yield and 99%ee.Meanwhile,this reduction reaction could be conducted on gram-scale without loss of activity and enantioselectivity,and the chiral ligand could be conveniently recovered with high yield.

关键词： Oxazole-pyrimidine ligands Planar chirality Nickel Hydroboration Asymmetric synthesis

Surface iodine and pyrenyl-graphdiyne co-modified Bi catalysts for highly efficient CO_(2) electroreduction in acidic electrolyte

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Nano Research 2024年第4期17卷 2381-2387页

作者： Min Zhang juan Wang Xin Rong Xiu-Li Lu Tong-Bu Lu MOE International Joint Laboratory of Materials Microstructure Institute for New Energy Materials and Low Carbon TechnologiesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China

CO_(2) electroreduction to formic acid/formate would contribute to alleviating the energy and climate crisis.This work reports a Bi-based catalyst derived from the in-situ electroreduction of Bi_(2)O_(2)CO_(3) modified with iodine and pyrenyl-graphdiyne(PGDY)on the surface for efficient electroreduction of CO_(2) in acidic electrolyte,with a high partial current density of 98.71 mA·cm^(-2) and high Faradaic efficiency(FE)>90%over the potential range from^(-1).2 to-1.5 V vs.reversible hydrogen electrode(RHE),as well as the long-term operational stability over 240 h without degradation in H-type cell.Experimental results and density function theory calculations show that the synergistic effect of surface iodine and PGDY is responsible for this active and extremely stable process of CO_(2) electroreduction via lowering the energy barriers for formation of*OCHO intermediate,suppressing the competitive HER by enhancing the concentration of both K+and CO_(2) at reaction interface,as well as preventing the dissolution and re-deposition of active Bi atoms on surface during catalytic reaction.This work provides new insight into designing highly active and stable electrocatalysts for CO_(2) reduction.

关键词： CO_(2) reduction electrocatalysis Bi-based catalysts acidic electrolyte

A Review on Engineering Transition Metal Compound Catalysts to Accelerate the Redox Kinetics of Sulfur Cathodes for Lithium–Sulfur Batteries

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Nano-Micro Letters 2024年第5期16卷 300-332页

作者： Liping Chen Guiqiang Cao Yong Li Guannan Zu Ruixian Duan Yang Bai Kaiyu Xue Yonghong Fu Yunhua Xu juan Wang Xifei Li Shaanxi Key Laboratory of Nanomaterials and Nanotechnology Xi’an University of Architecture and TechnologyXi’an 710055People’s Republic of China Institute of Advanced Electrochemical Energy and School of Materials Science and Engineering Xi’an University of TechnologyXi’an 710048People’s Republic of China Yulin University Yulin 719000People’s Republic of China School of Materials Science and Engineering Fuzhou UniversityFuzhou 350108People’s Republic of China

Engineering transition metal compounds(TMCs)catalysts with excellent adsorption-catalytic ability has been one of the most effec-tive strategies to accelerate the redox kinetics of sulfur cathodes.Herein,this review focuses on engineering TMCs catalysts by cation doping/anion doping/dual doping,bimetallic/bi-anionic TMCs,and TMCs-based heterostructure composites.It is obvious that introducing cations/anions to TMCs or constructing heterostructure can boost adsorption-catalytic capacity by regulating the electronic structure including energy band,d/p-band center,electron filling,and valence state.Moreover,the elec-tronic structure of doped/dual-ionic TMCs are adjusted by inducing ions with different electronegativity,electron filling,and ion radius,resulting in electron redistribution,bonds reconstruction,induced vacancies due to the electronic interaction and changed crystal structure such as lat-tice spacing and lattice distortion.Different from the aforementioned two strategies,heterostructures are constructed by two types of TMCs with different Fermi energy levels,which causes built-in electric field and electrons transfer through the interface,and induces electron redistribution and arranged local atoms to regulate the electronic structure.Additionally,the lacking studies of the three strategies to comprehensively regulate electronic structure for improving catalytic performance are pointed out.It is believed that this review can guide the design of advanced TMCs catalysts for boosting redox of lithium sulfur batteries.

关键词： Lithium–sulfur battery Redox kinetic Transition metal compounds catalyst Multiple metals/anions

A general synthetic strategy for N, P co-doped graphene supported metal-rich noble metal phosphides for hydrogen generation

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Green Energy & Environment 2024年第1期9卷 152-162页

作者： Jingwen Ma Xiang Li Guangyu Lei Jun wang juan Wang Jian Liu Ming Ke Yang Li Chunwen Sun School of Chemical and Environmental Engineering China University of Mining and Technology(Beijing)Beijing100083China State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing102249China Lab of Advanced Nano-structures&Transfer Processes Department of Chemical EngineeringTianjin UniversityTianjin300354China PetroChina Planning and Engineering Institute Beijing100083China

The exploitation of electrocatalysts with high activity and durability for HER is desirable for future energy systems,but it is still a challenge.NMPs have attracted increasing attentions,but the preparation process often needs toxic regents or dangerous reaction conditions.Herein,we develop a general green method to fabricate metal-rich NMPs anchored on NPG through pyrolyzing DNA cross-linked complexes.The obtained Ru_(2) P-NPG exhibits an ultrasmall overpotential of 7 mV at 10 mA cm^(2) and ultralow Tafel slope of 33 mV dec^(-1) in 1.0 mol L?1 KOH,even better than that of commercial Pt/C.In addition,Ru 2 P-NPG also shows low overpotentials of 29 and 78 mV in 0.5 mol L^(-1) H_(2)SO_(4) and 1.0 mol L^(-1) PBS,respectively.The superior activity can be attributed to the ultrafine dispersion of Ru 2 P nanoparticles for more accessible sites,more defects formed for abundant active sites,the two-dimensional plane structure for accelerated electron transfer and mass transport,as well as the regulation of electron distribution of the catalyst.Moreover,the synthetic method can also be applied to prepare other metal-rich noble metal phosphides(Pd_(3)P-NPG and Rh_(2)P-NPG),which also exhibits high activity for HER.This work provides an effective strategy for designing NMP-based electrocatalysts.

关键词： Noble metal phosphides Electrocatalyst Deoxyribonucleic acid Hydrogen evolution pH universal

Heterointerface engineering of assembled CoP_(2) on N-modified carbon as efficient trifunctional electrocatalysts for Zn-Air batteries and overall water splitting

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Nano Research 2024年第5期17卷 3801-3809页

作者： Yan Chen Zhenrui Yang juan Wang Yun Yang Xuedong He Yang wang Jiadong Chen Yaqing Guo Xin wang Shun wang Huile Jin Wenzhou Key Lab of Advanced Energy Storage and Conversion Zhejiang Province Key Lab of Leather EngineeringCollege of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China Zhejiang Engineering Research Center for Electrochemical Energy Materials and Devices Institute of New Materials and Industrial TechnologiesWenzhou UniversityWenzhou 325035China School of Chemical and Biomedical Engineering Nanyang Technological UniversitySingapore 637459Singapore

Enhancing catalytic activity through modulating the interaction between N-doped carbon and metal phosphides clusters is an effective approach.Herein,the electronic structure modulation of CoP_(2) supported N-modified carbon(CoP_(2)/NC)has been designed and prepared as efficient electrocatalysts for oxygen reduction reaction(ORR),oxygen evolution reaction(OER),and hydrogen evolution reaction(HER).Notably,CoP_(2)/NC-1 catalyst exhibits impressive performance in alkaline media,with an ORR half-wave potential of 0.84 V,as well as OER and HER overpotentials of 290 and 129 mV(at 10 mA·cm^(−2)),respectively.In addition,CoP_(2)/NC-1 produces a power density as high as 172.9 mW·cm^(−2),and excellent reversibility of 100 h at 20 mA·cm^(−2) in home-made Zn-air batteries.The experimental results demonstrate that the synergistic interactions between N modified carbon substrate and CoP_(2) material significantly enhance the kinetics of ORR,OER,and HER.Density functional theory(DFT)calculations reveal the strong electrons redistribution of CoP_(2) induced by high-density N atoms at the interface,thus optimizing the key intermediates and significantly lower the energy barrier of reactions.These electronic adjustments of CoP_(2) greatly enhance its kinetics of ORR/OER/HER,leading to faster reactions.This study provides profound insights into the specific modification of CoP_(2) by N-doped carbon,enabling the construction of efficient catalysts.

关键词： two-dimensional(2D)carbon metal-organic framework cobalt phosphide zinc air battery water splitting

Targeted nanostrategies eliminate pre-metastatic niche of cancer

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Nano Research 2024年第6期17卷 5358-5373页

作者： juan Wang Ning Zhang Xiuping Ding Chengrui Fu Xiaodong Li Baosheng Li Jianxun Ding Tianmeng Sun Key Laboratory of Organ Regeneration and Transplantation of Ministry of Education Institute of ImmunologyThe First HospitalJilin University1 Xinmin StreetChangchun 130061China Key Laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of Sciences5625 Renmin StreetChangchun 130022China Department of Radiation Oncology Shandong Cancer Hospital and InstituteShandong First Medical University and Shandong Academy of Medical Sciences440 Jiyan RoadJinan 250117China Department of orthopaedics The Second Hospital of Shandong UniversityShandong University247 Beiyuan StreetJinan 250033China State Key Laboratory of Molecular Engineering of Polymers Fudan University220 Handan RoadShanghai 200433China

Establishing a pre-metastatic niche(PMN)in secondary organs is a prerequisite for cancer metastases.Despite advances in cancer therapy,the efficient inhibition of PMN formation remains a clinical challenge.Recent advances in understanding the specific characteristics of PMN and advances in nanotechnology have provided hope for manipulating their microenvironments.A series of nanostrategies have been designed to eliminate the PMN,including the removal of pro-metastatic exosomes from the bloodstream for excretion via the intestines,the targeting and scavenging of myeloid-derived suppressor cells,fibroblasts,and critical extracellular matrix components,and the elimination of circulating tumor cells prior to colonization in distant organs.This review summarizes the underlying mechanisms of PMN formation,highlights the anti-PMN efficacy of currently reported nanostrategies,and underlines the unresolved questions.

关键词： nanoparticle controlled drug delivery pre-metastatic niche elimination metastasis suppression cancer therapy

Salsolinol as an RNA m~6A methylation inducer mediates dopaminergic neuronal death by regulating YAP1 and autophagy

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Neural Regeneration Research 2025年第3期20卷 887-899页

作者： Jianan wang Yuanyuan Ran Zihan Li Tianyuan Zhao Fangfang Zhang juan Wang Zongjian Liu Xuechai Chen Beijing International Science and Technology Cooperation Base for Antiviral Drugs College of Chemistry and LifeBeijing University of TechnologyBeijingChina Department of Rehabilitation Beijing Rehabilitation HospitalCapital Medical UniversityBeijingChina

Salsolinol(1-methyl-6,7-dihydroxy-1,2,3,4-tetrahydroisoquinoline,Sal)is a catechol isoquinoline that causes neurotoxicity and shares structural similarity with 1-methyl-4-phenyl-1,2,3,6-tetrahydropyridine,an environmental toxin that causes Parkinson's disease.However,the mechanism by which Sal mediates dopaminergic neuronal death remains unclear.In this study,we found that Sal significantly enhanced the global level of N~6-methyladenosine(m~6A)RNA methylation in PC12 cells,mainly by inducing the downregulation of the expression of m~6A demethylases fat mass and obesity-associated protein(FTO)and alk B homolog 5(ALKBH5).RNA sequencing analysis showed that Sal downregulated the Hippo signaling pathway.The m~6A reader YTH domain-containing family protein 2(YTHDF2)promoted the degradation of m~6A-containing Yes-associated protein 1(YAP1)mRNA,which is a downstream key effector in the Hippo signaling pathway.Additionally,downregulation of YAP1 promoted autophagy,indicating that the mutual regulation between YAP1 and autophagy can lead to neurotoxicity.These findings reveal the role of Sal on m~6A RNA methylation and suggest that Sal may act as an RNA methylation inducer mediating dopaminergic neuronal death through YAP1 and autophagy.Our results provide greater insights into the neurotoxic effects of catechol isoquinolines compared with other studies and may be a reference for assessing the involvement of RNA methylation in the pathogenesis of Parkinson's disease.

关键词： ALKBH5 autophagy FTO Hippo pathway m~6A Parkinson's disease RNA methylation salsolinol YAP1 YTHDF2

Lattice-distorted Pt wrinkled nanoparticles for highly effective hydrogen electrocatalysis

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Nano Research 2024年第5期17卷 3819-3826页

作者： Xue Li Xiang Han Zhenrui Yang Shun wang Yun Yang juan Wang Jiadong Chen Zhongwei Chen Huile Jin Wenzhou Key Lab of Advanced Energy Storage and Conversion Zhejiang Province Key Lab of Leather EngineeringCollege of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China Institute of New Materials and Industry Technology College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China Department of Chemical Engineering Waterloo Institute for NanotechnologyUniversity of WaterlooWaterlooOntario N2L 3G1Canada

Modulating Pt surfaces through the introduction of lattice distortion emerges as immensely effective strategy that enhances the kinetics of alkaline hydrogen evolution and oxidation processes.In this study,we fabricated lattice-distorted Pt wrinkled nanoparticles(LD-Pt WNPs)for efficient hydrogen electrocatalysis.The LD-Pt WNPs not only outperform the Pt/C benchmark in hydrogen oxidation reaction,achieving an excellent mass-specific current of 968.5 mA·mg_(Pt)^(-1)(9 times that of Pt/C),but also demonstrate outstanding hydrogen evolution reaction activity with a small overpotential of 58.0 mV.Comprehensive experiments and density functional theory calculations reveal that lattice defects introduce an abundance of unsaturated coordination atoms while modifying the d-band center of Pt.This dual effect optimizes the binding strength of crucial H and OH intermediates,leading to a significant reduction in the energy barrier of the reaction bottleneck,commonly known as the Volmer step.This work unveils a fresh viewpoint on projecting and developing high efficiency electrocatalysts through defect engineering.

关键词： distortion nanoparticle hydrogen evolution reaction defect engineering hydrogen oxidation reaction

Fine-mapping of a candidate gene for web blotch resistance in Arachis hypogaea L.

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Journal of Integrative Agriculture 2024年第5期23卷 1494-1506页

作者： Xiaohui Wu Mengyuan Zhang Zheng Zheng Ziqi Sun Feiyan Qi Hua Liu juan Wang Mengmeng wang Ruifang Zhao Yue Wu Xiao wang Hongfei Liu Wenzhao Dong Xinyou Zhang College of Agronomy Henan Agricultural UniversityZhengzhou 450046China Henan Academy of Agricultural Sciences/Henan Academy of Crop Molecular Breeding/Key Laboratory of Oil Crops in Huang-Huai-Hai Plain Ministry of Agriculture and Rural Affairs/Henan Provincial Key Laboratory for Oil Crop ImprovementZhengzhou 450002China The Shennong Laboratory Zhengzhou 450002China Shangqiu Academy of Agricultural and Forestry Sciences Shangqiu 476000China

Peanut(Arachis hypogaea L.)is a globally important oil crop.Web blotch is one of the most important foliar diseases affecting peanut,which results in serious yield losses worldwide.Breeding web blotch-resistant peanut varieties is the most effective and economically viable method for minimizing yield losses due to web blotch.In the current study,a bulked segregant analysis with next-generation sequencing was used to analyze an F2:3 segregating population and identify candidate loci related to web blotch resistance.Based on the fine-mapping of the candidate genomic interval using kompetitive allele-specific PCR(KASP)markers,we identified a novel web blotch resistance-related locus spanning approximately 169 kb on chromosome 16.This region included four annotated genes,of which only Arahy.35VVQ3 had a non-synonymous single nucleotide polymorphism in the coding region between the two parents.Two markers(Chr.16.12872635 and Chr.16.12966357)linked to this gene were shown to be co-segregated with the resistance of peanut web blotch by 72 randomly selected recombinant inbred lines(RIL),which could be used in marker-assisted breeding of resistant peanut varieties.

关键词： peanut web blotch bulked segregant analysis KAsP markers resistant gene

VSe_(2)/V_(2)C heterocatalyst with built-in electric field for efficient lithium-sulfur batteries:Remedies polysulfide shuttle and conversion kinetics

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Journal of Energy Chemistry 2024年第2期89卷 397-409,I0010页

作者： Yanwei Lv Lina Bai Qi Jin Siyu Deng Xinzhi Ma Fengfeng Han juan Wang Lirong Zhang Lili Wu Xitian Zhang Key Laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Physics and Electronic EngineeringHarbin Normal UniversityHarbin 150025HeilongjiangChina

Lithium sulfur(Li-S)battery is a kind of burgeoning energy storage system with high energy density.However,the electrolyte-soluble intermediate lithium polysulfides(Li PSs)undergo notorious shuttle effect,which seriously hinders the commercialization of Li-S batteries.Herein,a unique VSe_(2)/V_(2)C heterostructure with local built-in electric field was rationally engineered from V_(2)C parent via a facile thermal selenization process.It exquisitely synergizes the strong affinity of V_(2)C with the effective electrocatalytic activity of VSe_(2).More importantly,the local built-in electric field at the heterointerface can sufficiently promote the electron/ion transport ability and eventually boost the conversion kinetics of sulfur species.The Li-S battery equipped with VSe_(2)/V_(2)C-CNTs-PP separator achieved an outstanding initial specific capacity of 1439.1 m A h g^(-1)with a high capacity retention of 73%after 100 cycles at0.1 C.More impressively,a wonderful capacity of 571.6 mA h g^(-1)was effectively maintained after 600cycles at 2 C with a capacity decay rate of 0.07%.Even under a sulfur loading of 4.8 mg cm^(-2),areal capacity still can be up to 5.6 m A h cm^(-2).In-situ Raman tests explicitly illustrate the effectiveness of VSe_(2)/V_(2)C-CNTs modifier in restricting Li PSs shuttle.Combined with density functional theory calculations,the underlying mechanism of VSe_(2)/V_(2)C heterostructure for remedying Li PSs shuttling and conversion kinetics was deciphered.The strategy of constructing VSe_(2)/V_(2)C heterocatalyst in this work proposes a universal protocol to design metal selenide-based separator modifier for Li-S battery.Besides,it opens an efficient avenue for the separator engineering of Li-S batteries.

关键词： Li-S battery Shuttle effect Separator modifier VSe_(2)/V_(2)C heterostructure Built-in electric field