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Enhancing Green Ammonia Electrosynthesis Through Tuning Sn Vacancies in Sn‑Based MXene/ MAX Hybrids

Nano-Micro Letters 2024年第5期16卷 154-168页

作者： Xinyu Dai Zhen‑Yi Du Ying Sun Ping Chen Xiaoguang Duan Junjun Zhang Hui Li Yang Fu Baohua Jia Lei Zhang Wenhui Fang Jieshan Qiu Tianyi Ma Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning Province College of ChemistryInstitute of Clean Energy ChemistryLiaoning UniversityShenyang 110036People’s Republic of China State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024People’s Republic of China school of Chemistry and chemical Engineering Anhui UniversityHefei 230601People’s Republic of China school of chemical Engineering The University of AdelaideAdelaideSA 5005Australia State Key Laboratory of High‑Efficiency Utilization of Coal and Green chemical Engineering College of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021NingxiaPeople’s Republic of China school of Science RMIT UniversityMelbourneVIC 3000Australia Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640People’s Republic of China College of chemical Engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China

Renewable energy driven N_(2) electroreduction with air as nitrogen source holds great promise for realizing scalable green ammonia ***,relevant out-lab research is still in its ***,a novel Sn-based MXene/MAX hybrid with abundant Sn vacancies,Sn@Ti_(2)CTX/Ti_(2)SnC–V,was synthesized by controlled etching Sn@Ti_(2)SnC MAX phase and demonstrated as an efficient electrocatalyst for electrocatalytic N2 *** to the synergistic effect of MXene/MAX heterostructure,the existence of Sn vacancies and the highly dispersed Sn active sites,the obtained Sn@Ti2CTX/Ti_(2)SnC–V exhibits an optimal NH_(3) yield of 28.4μg h^(−1) mg_(cat)^(−1) with an excellent FE of 15.57% at−0.4 V versus reversible hydrogen electrode in 0.1 M Na_(2)SO_(4),as well as an ultra-long ***,this catalyst represents a satisfactory NH3 yield rate of 10.53μg h^(−1) mg^(−1) in the home-made simulation device,where commercial electrochemical photovoltaic cell was employed as power source,air and ultrapure water as feed *** as-proposed strategy represents great potential toward ammonia production in terms of financial cost according to the systematic technical economic *** work is of significance for large-scale green ammonia production.

关键词： Green ammonia synthesis N2 electroreduction Renewable energy Sn MXene/MAX hybrid

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A2B7-type La-Mg-Ni alloys prepared by Mg thermal diffusion for improved hydrogen storage performance

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Rare Metals 2024年第7期43卷 3260-3272页

作者： Yong-Xi Zhang Guan-Jiu Wu Jing Gu Hong-Xing Kang Yuan Li Di Zhou Wen-Feng Wang Lu Zhang Shu-Min Han Hebei Key Laboratory of Applied Chemistry School of Environmental and Chemical EngineeringYanshan University department of Chemistry and Biochemistry San Diego State University State Key Laboratory of Metastable Materials Science and technology Yanshan University

A novel approach based on thermal diffusion was used to achieve controllable Mg content in A2B7-type La-Mg-Ni-based *** formation mechanism of the A2B7-type phase as a result of the thermal diffusion process and the effect of Mg content on hydrogen storage performance were investigated.X-ray diffraction（XRD） patterns and Rietveld refinement results showed that increased Mg transformed the LaNi5phase in the La0.74Sm0.03Y0.23Ni4.32Al0.04precursor alloy into a superlattice *** electron microscopy（SEM） images showed that Mg was evenly distributed in the alloy *** in the superlattice significantly inhibited the phase decomposition of the superlattice structure during the hydrogen absorption/desorption *** A2B7-type La0.57Sm0.02Y0.18Mg0.23Ni3.38Al0.03alloy composed of Gd2Co7and Ce2Ni7phases was successfully *** pressure-composition isotherm profiles showed that the alloy had a hydrogen storage capacity as high as 1.73 wt%,with good cycling *** 50 cycles of hydrogen absorption/desorption,the alloy retained a hydrogen storage capacity of 1.45 wt%,with a capacity retention rate of up to 84.28%.The Mg thermal diffusion process thus provides a new approach for the controlled preparation of La-Mg-Ni-based alloys.

关键词： La–Mg–Ni-based hydrogen storage alloy A 2 B 7 -type superlattice alloy Mg thermal diffusion process Phase transformation Hydrogen storage property

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Catalytic activation of peroxodisulfate using shape-controlled cerium-manganese composite oxide for phenol degradation:Kinetics and degradation pathway investigation

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Journal of Rare Earths 2024年第8期42卷 1514-1523,I0004页

作者： Yanxia Zheng Lixi Yang Chuxin Huang Yuchao Li Cuncun Zuo Tingting Ge Haofei Huang Jiutao An Ming Wang Yansong Zhao Iinstitute of Clean chemical technology School of Chemistry and Chemical EngineeringShandong University of TechnologyZibo255000China Shandong Cllegial Enginering Rearch Center of Novel Rare Earth Catalys Materials Shandong University of TechnogyZibo255000 China College of Resources and Environment Engineering Shandong University of TechnologyZibo255000China department of Safety Chemistry and Biomedical Laboratory SciencesFaculty of Engineering and ScienceWestern Norway University of Applied Sciences(HVL)5063BergenNorway

Phenol-containing wastewater is typical organic wastewater,and its treatment is *** advanced method to treat this type of wastewater is persulfate *** friendly ceriummanganese composite oxide materials were synthesized by hydrothermal method and applied to the phenol degradation *** ratios of cerium and manganese,as well as the amount of sodium hydroxide,were *** solid solutions of cerium and manganese were formed and confirmed by X-ray diffraction(XRD) and transmission electron microscopy(TEM).H_(2)-temperature programmed reduction(H_(2)-TPR) and X-ray photoelectron spectroscopy(XPS) were utilized to analyze the synergistic effect of cerium and *** is found that there is a transformation between Ce^(4+)/Ce^(3+) and Mn^(2+)/Mn^(3+),which makes the material more trivalent manganese and thereby increases the catalytic *** effect of materials in catalyzing phenol degradation by peroxodisulfate(PDS) under various preparation conditions is discussed and high-effciency removal of phenol can be achieved and the removal rate at 180 min is close to 100%.The kinetic of this process was investigated and activation energy of phenol degradation is 62,35 kJ/*** degradation pathway of phenol was studied and it is found that PDS can be activated by low metal ions and the OH and SO_(4·)^(-)radicals play crucial roles according to the quenching experiments.

关键词： Advanced oxidation process Persulfate Mn-Ce solid solution Phenol degradation Rare earths

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Atomically dispersed Mn-N_(x) catalysts derived from Mn-hexamine coordination frameworks for oxygen reduction reaction

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Carbon Energy 2024年第5期6卷 114-126页

作者： Guoyu Zhong Liuyong Zou Xiao Chi Zhen Meng Zehong Chen Tingzhen Li Yongfa Huang Xiaobo Fu Wenbo Liao Shaona Zheng Yongjun Xu Feng Peng Xinwen Peng Guangdong Provincial Key Laboratory of Distributed Energy Systems School of Chemical Engineering and Energy TechnologyDongguan University of TechnologyDongguanChina State Key Laboratory of Pulp and Paper Engineering South China University of TechnologyGuangzhouChina department of Chemistry Centre for Advanced 2D Materials(CA2DM)National University of SingaporeSingaporeSingapore school of Chemistry and chemical Engineering Guangzhou UniversityGuangzhouChina

Metal-organic frameworks recently have been burgeoning and used as precursors to obtain various metal-nitrogen-carbon catalysts for oxygen reduction reaction(ORR).Although rarely studied,Mn-N-C is a promising catalyst for ORR due to its weak Fenton reaction activity and strong graphitization ***,we developed a facile strategy for anchoring the atomically dispersed nitrogen-coordinated single Mn sites on carbon nanosheets(MnNCS)from an Mn-hexamine coordination *** atomically dispersed Mn-N_(4) sites were dispersed on ultrathin carbon nanosheets with a hierarchically porous *** optimized MnNCS displayed an excellent ORR performance in half-cells(0.89 V *** hydrogen electrode(RHE)in base and 0.76 V *** in acid in half-wave potential)and Zn-air batteries(233 mW cm^(−2)in peak power density),along with significantly enhanced *** functional theory calculations further corroborated that the Mn-N_(4)-C(12)site has favorable adsorption of*OH as the rate-determining *** findings demonstrate that the metal-hexamine coordination framework can be used as a model system for the rational design of highly active atomic metal catalysts for energy applications.

关键词： carbon nanosheets electrocatalyst metal-organic frameworks Mn-N_(4) oxygen reduction reaction Zn-air batteries

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An efficient molten-salt electro-deoxidation strategy enabling fast-kinetics and long-life aluminum-selenium batteries

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SusMat 2024年第1期4卷 126-139页

作者： Jiguo Tu Zheng Huang Cheng Chang Haiping Lei Shuai Wang Shuqiang Jiao State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijingChina school of Chemistry Chemical Engineering and BiotechnologyNanyang Technological UniversitySingaporeSingapore school of Metallurgical and Ecological Engineering University of Science and Technology BeijingBeijingChina school of Electrical and Electronic Engineering Nanyang Technological UniversitySingaporeSingapore

Aluminum-selenium(Al-Se)batteries have been considered as one of the most promising energy storage systems owing to their high capacity,energy density,and cost effectiveness,but Se falls challenges in addressing the shuttle effect of soluble intermediate product and sluggish reaction kinetics in the solid-solid conversion process during ***,we propose an unprecedented design concept for fabricating uniform Se/C hollow microspheres with controllable morphologies through low-temperature electro-deoxidation in neutral NaCl-AlCl_(3) molten salt *** Se/C hollow microspheres are demonstrated to hold a favorable hollow structure for hosting Se,which can not only suppress the dissolution of soluble intermediate products into the electrolyte,thereby maintaining the structural integrity and maximizing Se utilization of the active material,but also promote the electrical/ionic conductivity,thus facilitating the rapid reaction kinetics during ***,the as-prepared Se/C hollow microspheres exhibit a high reversible capacity of 720.1 mAh g^(−1)at 500 mA g^(−1).Even at the high current density of 1000 mA g^(−1),Se/C delivers a high discharge capacity of 564.0 mAh g^(−1),long-term stability over 1100 cycles and high Coulombic efficiency of 98.6%.This present work provides valuable insights into short-process recovery of advanced Se-containingmaterials and value-added utilization for energy storage.

关键词： aluminum-ion batteries hollow Se/C microspheres long-term cycling stability lowtemperature electro-deoxidation NaCl-AlCl_(3)molten salt

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Metal and ligand modification modulates the electrocatalytic HER,OER,and ORR activity of 2D conductive metal-organic frameworks

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Nano Research 2024年第9期17卷 7984-7990页

作者： Yanan Zhou Li Sheng Lanlan Chen Wenhui Zhao Wenhua Zhang Jinlong Yang school of Material Science and chemical Engineering Institute of Mass SpectrometryNingbo UniversityNingbo 315211China department of chemical Physics University of Science and Technology of ChinaHefei 230026China department of Material Science and Engineering University of Science and Technology of ChinaHefei 230026China department of Physics Ningbo UniversityNingbo 315211China Hefei National Laboratory for Physical Sciences at the Microscale CAS Key Laboratory of Materials for Energy Conversion and Synergetic Innovation Centre of Quantum Information and Quantum PhysicsUniversity of Science and Technology of ChinaHefei 230026China

It is highly desirable to design efficient and stable hydrogen evolution reaction(HER)and oxygen evolution/reduction reaction(OER/ORR)electrocatalysts for the development of renewable energy ***,density functional theory(DFT)calculations were conducted to systematically investigate a series of TMN_(x)O_(4-x)-HTT(TM=Fe,Co,Ni,Ru,Rh,Pd,Ir and Pt;HTT=hexahydroxy tetraazanaphthotetraphene)analogs of two-dimensional(2D)conductive metal-organic frameworks(MOFs)as potential electrocatalysts for the HER,OER and *** thermodynamic and electrochemical stability simulations suggest that these designed catalysts are ***,CoO_(4)-HTT,RhN_(3)O_(1)-HTT and IrN3O1-HTT are predicted to be the most promising catalysts for the HER,OER and ORR,respectively,surpassing the catalytic activity of corresponding benchmark *** volcano plots were established based on the scaling relationship of adsorption Gibbs free energy of *** results reveal that regulating combinations of metal active centers and local coordination environments could effectively balance the interaction strength between intermediates and catalysts,thus achieving optimal catalytic *** findings not only opt for the promising HER/OER/ORR electrocatalysts but also guide the design of efficient electrocatalysts based on 2D MOFs materials.

关键词： hydrogen evolution reaction(HER) oxygen evolution/reduction reaction(OER/ORR) electrocatalysts design twodimensional(2D)conductive metal-organic frameworks(MOFs) density functional theory(DFT)

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Hard-carbon hybrid Li-ion/metal anode enabled by preferred mesoporous uniform lithium growth mechanism

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Journal of Energy Chemistry 2024年第1期88卷 252-259,I0006页

作者： Fang Yan Yan Liu Yuan Li Yan Wang Zicen Deng Meng Li Zhenwei Zhu Aohan Zhou Ting Li Jingyi Qiu Gaoping Cao Shaobo Huang Biyan Wang Hao Zhang school of Chemistry and Biological Engineering University of Science and TechnologyBeijing 100083China Research Institute of chemical Defense Beijing 100191China College of Physics and Engineering Henan University of Science and TechnologyLuoyang 471023HenanChina National Base for International Science&technology Cooperation School of ChemistryXiangtan UniversityXiangtan 411105HunanChina Materials and Manufacturing department Beijing University of TechnologyBeijing 100124China

To achieve high energy density in lithium batteries,the construction of lithium-ion/metal hybrid anodes is a promising *** particular,because of the anisotropy of graphite,hybrid anode formed by graphite/Li metal has low transport kinetics and is easy to causes the growth of lithium dendrites and accumulation of dead Li,which seriously affects the cycle life of batteries and even causes safety ***,by comparing graphite with two types of hard carbon,it was found that hybrid anode formed by hard carbon and lithium metal,possessing more disordered mesoporous structure and lithophilic groups,presents better *** indicate that the mesoporous structure provides abundant active site and storage space for dead *** the synergistic effect of this structure and lithophilic functional groups(–COOH),the reversibility of hard carbon/lithium metal hybrid anode is maintained,promoting uniform deposition of lithium metal and alleviating formation of lithium *** hybrid anode maintains a 99.5%Coulombic efficiency(CE)after 260 cycles at a specific capacity of 500 m Ah/*** work provides new insights into the hybrid anodes formed by carbon-based materials and lithium metal with high specific energy and fast charging ability.

关键词： Hard carbon/Li metal hybrid anode Mesoporous structure Surface oxygen functional group Fast charging Lithium batteries

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Amino-functionalized UiO-66-doped mixed matrix membranes with high permeation performance and fouling resistance

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Chinese Journal of chemical Engineering 2024年第3期67卷 68-77页

作者： Yi Zhang Di Liu Zhaoli Wang Junjian Yu Yanyin Cheng Wenjing Li Zhe Wang Hongzhe Ni Yuchao Wang school of chemical Engineering Changchun University of TechnologyChangchun 130012China Advanced Institute of Materials Science Changchun University of TechnologyChangchun 130012China Key Laboratory of Advanced Functional Polymer Membrane Materials of Jilin Province Changchun 130012China school of Chemistry and Life Science Changchun University of TechnologyChangchun 130012China

For the reduction of bovine serum proteins from wastewater,a novel mixed matrix membrane was prepared by functionalizing the substrate material polyaryletherketone(PAEK),followed by carboxyl groups(C-SPAEKS),and then adding amino-functionalized UiO-66-NH_(2)(Am-UiO-66-NH_(2)).Aminofunctionalization of UiO-66 was accomplished by melamine,followed by an amidation reaction to immobilize Am-UiO-66-NH_(2),which was immobilized on the surface of the membrane as well as in the pore channels,which enhanced the hydrophilicity of the membrane surface while increasing the negative potential of the membrane *** nanoparticle-loaded ultrafiltration membrane has good permeation performance,with a pure water flux of up to 482.3 L·m^(-2)·h^(-1) for C-SPAEKS/AmUiO-66-NH_(2) and a retention rate of up to 98.7%for bovine serum albumin(BSA)-contaminated ***,after several hydrophilic modifications,the flux recovery of BSA contaminants by this series of membranes increased from 56.2%to 80.55%of pure *** results of ultra-filtration flux time tests performed at room temperature showed that the series of ultrafiltration membranes remained relatively stable over a test time of 300 ***,the newly developed mixed matrix membrane showed potential for high efficiency and stability in wastewater treatment containing bovine serum proteins.

关键词： Ultrafiltration Mixed matrix membranes Amino functionalization Hydrophilic modification Negatively charged

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Photo-controllable antifouling hydrogels embedded with AgNPs coated spiropyran functionalized mesoporous silica for long-term antibacterial activity

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Nano Research 2024年第9期17卷 8337-8349页

作者： Wei Su Fei Wang Bing Chen Ruoke Li Jindian Liu Junjie Xu Jianhua Fan Yueling Liu State Key Laboratory of Bioreactor Engineering East China University of Science and TechnologyShanghai 200237China department of Applied Biology School of BiotechnologyEast China University of Science and TechnologyShanghai 200237China

Silver nanoparticles(AgNPs)are widely used in antimicrobial ***,its easy aggregation and rapid loss hinder the effective *** address this issue,a novel stimuli-responsive antibacterial nanocomposite(Ag@SP-MSN)was developed based on spiropyran covalently conjugated mesoporous silica nanoparticles(284.6 nm)and AgNPs(27.1 nm)via strong electrostatic *** transmission electron microscopy(TEM)and atomic force microscopy(AFM)images proved the successful modification of AgNPs onto *** light-induced maximum loading amount towards AgNPs was calculated to be 95.0 wt.%after ultraviolet irradiation,while the amount of AgNPs released from Ag@SP-MSN was 94.4 wt.%under visible light in the aid of ammonia(0.1%,v/v).Upon cycled light irradiation,Ag@SP-MSN could recover 84.5 wt.%of AgNPs even after four *** proposed Ag@SP-MSN exhibited better antibacterial activity against both *** and *** than Ag@MSN under visible light illumination,indicating the efficient photo-responsive isomerization of ***,the Ag@SP-MSN embedded gel demonstrated outstanding antifouling ability even after 21 days when compared to AgNPs *** long-term photo-controllable antifouling property proved the excellent reversible absorption and release of Ag@SP-MSN towards *** work provides new insights into the safe utilization of nanomaterials,offering promising advancements to meet clinical antibacterial requirements.

关键词： light-responsive silver nanoparticles spiropyran mesoporous silica nanoparticles antibacterial activity

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Cation-πinteractions regulate electrocatalytic water oxidation over iridium single atoms supported on conjugated polymers

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Science China Chemistry 2024年第6期67卷 2063-2069页

作者： Jing Bai Yunxia Liu Ziwei Ma Shouhan Zhang Guojie Chao Haiping Lin Elke Debroye Longsheng Zhang Tianxi Liu Key Laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi214122China school of Chemistry and chemical Engineering Northwestern Polytechnical UniversityXi’an710072China school of Physics and Information technology Shanxi Normal UniversityXi’an710062China department of Chemistry KU LeuvenCelestijnenlaan 200FLeuven3001Belgium

Designing cost-effective and high-performing metal catalysts is significant for many renewable energy conversion *** metal loading without sacrificing activity and durability is highly desired for the catalyst design,especially for those reactions where the noble metals deliver the best catalyzing ***-atom catalysts(SACs)with maximal metalatom utilization,homogeneous and tailorable active sites have emerged as promising catalyst candidates,where the local coordination structures of the metal atoms in SACs largely determine the reaction *** design strategies of constructing strong metal-support interactions can stabilize the individual metal atoms in SACs,but present obstacles to provide a flexible manipulation platform for elaborately tailoring the coordination structures to achieve performance optimization towards a specifically targeted ***,for the proof-of-concept study,we report a novel design of SAC with iridium(Ir)single atoms supported on conjugated polymer,in which the adsorption energies of reaction intermediates on Ir atoms and the reaction kinetics towards acidic water oxidation can be readily optimized through modulating the formed cation-πinteractions that can be tailored by adjusting the molecular structures of conjugated *** strategy establishes a general route to develop targeted SACs for various catalytic reactions.

关键词： conjugated polymers single-atom catalysts cation-πinteractions oxygen evolution reaction

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