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Boosting Electrochemical Urea Synthesis via Constructing Ordered Pd–Zn Active Pair

Nano-Micro Letters 2024年第11期16卷 529-540页

作者： Weiliang Zhou Chao Feng Xuan Li Xingxing Jiang Lingyan Jing Shuai Qi Qihua Huo Miaoyuan Lv Xinbao Chen Tianchi Huang Jingwen Zhao Na Meng Hengpan Yang Qi Hu Chuanxin He College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060GuangdongPeople’s Republic of China School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering Shihezi UniversityShihezi 832003XinjiangPeople’s Republic of China

Electrochemical co-reduction of nitrate(NO_(3)^(-))and carbon dioxide(CO_(2))has been widely regarded as a promising route to produce urea under ambient conditions,however the yield rate of urea has remained ***,we report an atomically ordered intermetallic pallium-zinc(PdZn)electrocatalyst comprising a high density of PdZn pairs for boosting urea *** is found that Pd and Zn are responsible for the adsorption and activation of NO_(3)^(-)and CO_(2),respectively,and thus the co-adsorption and co-activation NO_(3)^(-)and CO_(2) are achieved in ordered PdZn *** importantly,the ordered and well-defined PdZn pairs provide a dual-site geometric structure conducive to the key C-N coupling with a low kinetical barrier,as demonstrated on both operando measurements and theoretical ***,the PdZn electrocatalyst displays excellent performance for the co-reduction to generate urea with a maximum urea Faradaic efficiency of 62.78%and a urea yield rate of 1274.42μg mg^(-1) h^(-1),and the latter is 1.5-fold larger than disordered pairs in PdZn *** work paves new pathways to boost urea electrosynthesis via constructing ordered dual-metal pairs.

关键词： Electrochemical C-N coupling Urea electrosynthesis Intermetallic compounds Geometric structures Active pairs

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Heterostructuring 2D Co_(2)P nanosheets with 0D CoP via a saltassisted strategy for boosting hydrogen evolution from ammonia borane hydrolysis

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Nano Research 2023年第5期16卷 6260-6269页

作者： Chao Wan Xiaoling Liu Jiapei Wang Fengqiu Chen Dang-Guo Cheng Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China School of Chemistry and Chemical Engineering Anhui University of TechnologyMa’anshan 243002China

Ammonia borane(NH3BH3,AB)holds promise for chemical storage of ***,designing superb and low-cost photocatalyst to drive hydrogen evolution from AB under visible light irradiation is highly desirable but remains a major challenge for promoting the practical utilization of ***,we demonstrated a heterostructure photocatalyst consisting of zerodimensional(0D)CoP nanoparticles immobilized on two-dimensional(2D)Co_(2)P nanosheets(CoP/Co_(2)Ps)as a high-performance and low-cost catalyst for hydrogen evolution from AB hydrolysis,in which 0D/2D heterostructure was synthesized using the saltinduced phase transformation ***,the optimized CoP/Co_(2)Ps exhibit a robust H_(2) evolution rate of 32.1 L∙min^(−1)∙g_(Co)^(−1),corresponding to a turnover frequency(TOF)value of 64.1 min^(−1),being among the highest TOF for non-noblemetal catalysts ever reported,even outperforming some precious metal *** work not only opens a new avenue to accelerate hydrogen evolution from AB by regulating the electronic structures of heterointerfaces,but also provides a novel strategy for the construction of precious-metal-free materials for hydrogen-related energy catalysis in the future.

关键词： hydrogen storage ammonia borane hydrolysis heterostructure CoP/Co_(2)P nanosheets(CoP/Co_(2)Ps) hydrogen evolution

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A multifunctional electrolyte additive for zinc-ion capacitors with low temperature resistant and long lifespan

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Journal of Energy Chemistry 2024年第7期94卷 477-485页

作者： Ming Sun Zekai Zhang Shuqing Fu Yifan Zhang Ruoyu Wang Hongchun Mu Cheng Lian Wenqiang Wang Gengchao Wang Shanghai Engineering Research Center of Hierarchical Nanomaterials Shanghai Key Laboratory of Advanced Polymeric MaterialsSchool of Materials Science and EngineeringEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Chemical Engineering Shanghai Engineering Research Center of Hierarchical NanomaterialsFrontiers Science Center for Materiobiology and Dynamic Chemistryand School of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200438China

Aqueous zinc-ion capacitors (ZICs) are considered as potential candidates for next generation electrochemical energy storage devices due to their high safety and low ***,the existing aqueous ZICs usually have the problems of zinc dendrite growth and unsatisfactory performance at low ***,an erythritol (Eryt) additive with inhibition of zinc dendrites and anti-freezing capability was introduced into the *** experimental characterization and theoretical calculation confirm that the Eryt adsorbed on the surface of zinc anodes regulates the deposition orientation of Zn^(2+) and inhibits the formation of *** also reconstructs the solvation structure in the electrolyte to reduce water activity,enabling the electrolyte to have a lower freezing point for operation at low *** the assistance of Eryt,the Zn||Zn symmetric cell exhibits a long cycle life of 2000 h,while the ZIC assembled with activated carbon (AC) cathode and zinc anode (Zn||AC) maintains a capacity retention of 98.2% after 30,000 cycles at a current density of 10 A g^(-1)(even after 10,000 cycles at-20°C,the capacity retention rate reached 94.8%.).This work provides a highly scalable,low-cost and effective strategy for the protection of the anodes of low-temperature aqueous ZICs.

关键词： Zinc-ioncapacitors Electrolyte additive Dendrite-free Freeze-resistant electrolyte

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Preparation of carbon nanotube films towards mechanical and electrochemical energy storage

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Nano Research 2023年第11期16卷 12411-12429页

作者： Yukang Zhu Yanbin Wei Zhenxing Zhu Hongjie Yue Ziying He Qi Zhang Shijun Zhang Fei Wei Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Beijing Research Institute of Chemical Industry SINOPECBeijing 100013China

Due to unique and excellent properties,carbon nanotubes(CNTs)are expected to become the next-generation critical engineering mechanical and energy storage materials,which will play a key role as building blocks in aerospace,military equipment,communication sensing,and other cutting-edge *** practical application,the assembled macrostructures from individual CNTs are the common paradigms such as fibers or *** the main representative,CNT films can not only retain the unique properties of their CNTs components,but also are more likely for mass-production than other ***,in this review,we focus on preparation of CNT films and discuss their emerging applications in the field of mechanical and electrochemical energy storage/***,different preparation processes are systematically *** we introduce some typical strategies to improve their mechanical performances besides strengthening *** on the progress of mass-production and performance optimization,we further discuss their potential utilization in mechanical and electrochemical energy storage/conversion ***,future perspectives for the development of CNT films in both production and application are *** hope that this review will shed light on the preparation/assembly of CNT films and integrated application of excellent properties from individual to macroscopic ***,the preparation and cross-scale application paradigms of CNT films also offer a good model for other macroscopic ordered assemblies of one-dimensional nanomaterials.

关键词： carbon nanotubes carbon nanotube film preparation mechanical strengthening energy storage

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Immobile polyanionic backbone enables a 900-μm-thick electrode for compact energy storage with unprecedented areal capacitance

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National Science Review 2024年第8期11卷 209-218页

作者： Haoran Li Zhitan Wu Xiaochen Liu Haotian Lu Weichao Zhang Fangbing Li Hongyuan Yu Jinyang Yu Boya Zhang Zhenxin Xiong Ying Tao Quan-Hong Yang Nanoyang Group Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy StorageSchool of Chemical Engineering and Technology National Industry-Education Integration Platform of Energy Storage and Collaborative Innovation Center of Chemical Science and Engineering Tianjin University Haihe Laboratory of Sustainable Chemical Transformations Joint School of the National University of Singapore and Tianjin University International Campus of Tianjin University

Thickening of electrodes is crucial for maximizing the proportion of active components and thus improving the energy density of practical energy storage ***,trade-offs between electrode thickness and electrochemical performance persist because of the considerably increased ion transport resistance of thick ***,we propose accelerating ion transport through thick and dense electrodes by establishing an immobile polyanionic backbone within the electrode pores;and as a proof of concept,gel polyacrylic electrolytes as such a backbone are in situ synthesized for *** charge and discharge,protons rapidly hop among RCOO-sites for oriented transport,fundamentally reducing the effects of electrode tortuosity and polarization resulting from concentration ***,nearly constant ion transport resistance per unit thickness is achieved,even in the case of a 900-μm-thick dense electrode,leading to unprecedented areal capacitances of 14.85 F cm-2at 1 mA cm-2and 4.26 F cm-2at 100 mA *** study provides an efficient method for accelerating ion transport through thick and dense electrodes,indicating a significant solution for achieving high energy density in energy storage devices,including but not limited to supercapacitors.

关键词： gel polymer electrolyte thick electrode ion transport areal capacitance compact energy storage

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Rational cathode configuration with bilayer membranes to engineer current-collector-free high-areal-sulfur lithium-sulfur batteries

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Nano Research 2024年第6期17卷 5224-5232页

作者： Jianmei Han Hua Zhang Peng Wang Ning Song Xuguang An Baojuan Xi Shenglin Xiong College of Chemistry and Chemical Engineering Taishan UniversityTai’an 271021China Key Laboratory of the Colloid and Interface Chemistry Ministry of Educationand School of Chemistry and Chemical EngineeringShandong UniversityJinan 250100China School of Mechanical Engineering Chengdu UniversityChengdu 610106China

The application of light-weight current collectors is preferred because of the increased energy density of the *** it in mind,the cathode is designed with self-made paperlike memberane as current collector coupled with another interlayer to enable the high-energy-density lithium-sulfur *** a facile and green step-by-step methodology,the hybrid membrane is finalized successfully,consisting of reduced graphene oxide sheets covering paper-derived carbon(GPC)bearing Fe@Fe2O3 and Fe1−xS@Fe2O3 core-shell nanoparticles(FeFeO/FeSFeO@GPC).The film works as the current collector and interlayer simultaneously considering the porous and conductive *** demonstrated by the electrochemical testing,the FeFeO/FeSFeO@GPC hybrid cell exhibits attractive cycling stability and superior rate *** cell configuration and structural/composition merits of FeFeO/FeSFeO@GPC film facilitate the faster reaction kinetics,conducive to the improvement of capacity *** view of the effective cathode design,the areal sulfur loading is increased to 10.46 mg·cm^(−2)and a reversible capacity of 6.67 mAh·cm^(−2)can be retained after 60 cycles at 0.1 C.

关键词： light-weight self-made current collector core-shell high-areal-sulfur lithium-sulfur batteries

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Hyperbranched polyborosilazanes derived SiBCN ceramic for high-temperature wave-transparent performance

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Journal of Materials Science & technology 2024年第29期196卷 162-170页

作者： Zhen Yu Mingwei Ma Ziyu Liu Zhengyi Zhang Chunjia Luo Tiantian Zhang Jie Kong MOE Key Laboratory of Materials Physics and Chemistry in Extraordinary Conditions Shaanxi Key Laboratory of Macromolecular Science and TechnologySchool of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an 710072China School of Materials Science and Engineering Chang’an UniversityXi’an 710064China

Polymer-derived ceramics(PDCs)is a promising way to prepare ceramic-based electromagnetic functional materials,which can conveniently modulate the composition and dielectric properties of the *** this paper,SiBCN ceramic matrix composites with excellent high-temperature wave-transparent performance were prepared through PDC *** hyperbranched polyborosilazanes(PBSZs)were prepared by adjusting the type of chlorosilane monomers containing different numbers of methyl *** carbon element of pyrolytic ceramics was tuned by adjusting the molecular structure of the precursor and the pyrolysis *** lower the methyl number and pyrolysis temperature,the lower the dielectric constant of the polymer-derived SiBCN ceramics,which is favorable for electromagnetic wave(EMW)*** average EMW transmittance of SiBCN-C pyrolyzed from hyperbranched PBSZ using trichlorosilane at 1000℃ was 90.56%at room *** excitingly,the excellent wave-transparent performance was also maintained in the temperature range of 100-800℃.At the test temperature of 800℃,SiBCN-C-1000 still had excellent wave-transparent performance with minimum and average EMW transmittance of 76.13%and 88.96%,*** paper provided a new idea for the preparation of high-temperature wave-transparent SiBCN composite ceramics.

关键词： Polymer-derived ceramic SiBCN Low carbon content High temperature wave-transparent materials

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Fluoride ions adsorption from water by CaCO_(3)enhanced Mn-Fe mixed metal oxides

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Frontiers of chemical Science and engineering 2023年第2期17卷 236-248页

作者： Xinyuan Wang Heriberto Pfeiffer Jiangjiang Wei Jinyu Wang Jinli Zhang School of Chemistry and Chemical Engineering/Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan Shihezi UniversityShihezi 832003China Institute of Materials National Autonomous University of MexicoMexico City 04510Mexico School of Chemical Engineering and Technology Tianjin UniversityTianjin 300350China

Novel CaCO_(3)-enhanced Mn-Fe mixed metal oxides(CMFC)were successfully prepared for the first time by a simple-green hydrothermal strategy without any surfactant or template combined with calcination *** oxides were then employed as an adsorbent for adsorptive removal of excess fluoride *** adsorbent was characterized by SEM,XPS,XRD,FTIR,and BET analysis *** adsorption property of CMFC toward fluoride ion was analyzed by batch *** fact,CMFC exhibited adsorption capacity of 227.3 mg∙g^(-1)toward fluoride *** showed that ion exchange,electrostatic attraction and chemical adsorption were the main mechanism for the adhesion of large amount of fluoride ion on the CMFC surface,and the high adsorption capacity responded to the low pH of the adsorption *** the fluoride ion concentration was increased from 20 to 200 mg∙L^(-1),Langmuir model was more in line with experimental *** change of fluoride ion adsorption with respect to time was accurately described by pseudosecond-order *** five cycles of use,the adsorbent still maintains a performance of 70.6%of efficiency,compared to the fresh ***,this material may act as a potential candidate for adsorbent with broad range of application prospects.

关键词： mesoporous materials metal oxides fluoride ion adsorption mechanism

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Palladium-Catalyzed Tandem Cyclization Strategy for the Assembly of 3-Halo-1,2,5-triarylpyrroles from N-Alkylanilines and Haloalkynes

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Chinese Journal of Chemistry 2023年第2期41卷 181-187页

作者： Songjia Fang Huanfeng Jiang Wanqing Wu Key Laboratory of Functional Molecular Engineering of Guangdong Province State Key Laboratory of Luminescent Materials and DevicesSchool of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhouGuangdong 510640China

This report discloses a distinctive palladium-catalyzed sequential tandem cyclization reaction of two molecular haloalkynes and one molecular N-alkylanilines,leading to the efficient assembly of various 3-halo-1,2,5-triarylpyrrole *** carbon-carbon tri-ple bonds and one carbon-halogen bond in two molecular haloalkynes are transformed conveniently in one single step,which may involve the aminoalkynylation of haloalkyne and cyclization of the newly formed enyne *** high chemo-and regiose-lectivities,good functional group tolerance and late-stage modification of the halopyrrole products further illustrate the synthetic value of this strategy.

关键词： Palladium-catalyzed Haloalkynes N-Alkylanilines Cyclization Halopyrroles Amines Insertion Synthetic methods

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Understanding the cooperative effects in the catalysis of homodimeric fluoroacetate dehalogenase

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Science China Chemistry 2024年第7期67卷 2382-2391页

作者： Ke-Wei Chen Jia-Nan Chen Jun Zhang Chao Wang Tian-Yu Sun Yun-Dong Wu Key Laboratory of Computational Chemistry and Drug Design State Key Laboratory of Chemical OncogenomicSchool of Chemical Biology and BiotechnologyPeking University Shenzhen Graduate SchoolShenzhen 518055China Institute of Chemical Biology Shenzhen Bay LaboratoryShenzhen 518132China College of Chemistry and Molecular Engineering Peking UniversityBeijing 100871China Changping Laboratory Beijing 102200China

Fluoroacetate dehalogenases(FAcD),a homodimeric enzyme,catalyzes the conversion of fluoroacetic acid to glycolic acid(GoA).It has been proved that the enzyme has a half-of-the-site ***,its catalytic(C)subunit converts the first substrate to a covalent intermediate;then,the non-catalytic(NC)subunit binds a second substrate and promotes the conversion of the intermediate in the C subunit into the final *** the release of the product,the C subunit becomes the NC subunit,and the previous NC subunit becomes the C *** elucidate the detailed mechanism behind this cooperative catalysis,we have conducted microsecond-scale MD simulations along the reaction *** simulations indicate that the substrate in the NC subunit induces W185 and Y141 adopting an open conformation in the C *** opening of W185(C)facilitates the entry of catalytic water,enhancing the catalytic activity for product formation,while the opening of Y141(C)creates an unfavorable environment for product binding,promoting its *** interaction network analysis reveals that the substrate in the NC subunit can induce conformational changes through a conserved water chain at the interface.

关键词： enzyme catalysis molecular dynamics cooperative effect pre-reaction state

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