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Elucidating and manipulating pressure-induced water intrusion–extrusion in tunable hydrophobic Co/Zn bimetallic ZIFs:Roles of pore size and hydrogen bond

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Nano Research 2024年第1期17卷 344-353页

作者： Diyi Fang Chuanlei Liu Yu Chen Qilong Peng Kongguo Wu Yuxiang Chen Hao Jiang Yuan Wu Benxian Shen Qiumin Wu Di Wu Hui Sun International Joint Research center of green energy chemical engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China Alexandra Navrotsky Institute for Experimental Thermodynamics The Gene and Linda Voiland School of Chemical Engineering and BioengineeringMaterials Science and Engineeringand Department of ChemistryWashington State UniversityWashington 99163USA

Porous heterogeneous lyophobic systems(HLSs)find potential applications in energy restoring,dissipating,and ***,the development of controllable HLSs still lacks rational structure design of nanoporous materials matching the molecular sizes of adopted *** that,thoroughly understanding the underlying transportation mechanism in the confined nano channels is greatly *** this work,a series of Co/Zn bimetallic zeolitic imidazolate frameworks(ZIFs)with tunable structures were synthesized via regulating the Co to Zn ratios and employed to investigate the intrusion–extrusion of liquid water in confined *** characterizations confirm the heterometallic coordination in the Co/Zn-doped *** intrusion–extrusion experiments unlock the relationship between the intrusion pressure and the nanopore size and realize the evolution of the HLSs between molecular spring and *** addition,cycling tests indicate the reversible structure change of Co/Zn ZIFs encountering pressure-induced water *** combination with molecular dynamics simulations,we present that the water multimers intrude into nanopores of ZIFs in chain-like forms along with dissociation of hydrogen bonds(HBs).Water molecules in the pre-intrusion state exhibit reduced HBs in response to the increase of pressure and linear structure with 1.6–3.0 HBs on *** transition to the post-intrusion situation,the associative configuration of water tends to exhibit the tetrahedral ***,we highlight the roles of pore size and HB in synergically dominating the pressure-induced intrusion–extrusion of liquid water in hydrophobic ***,the present work can also guide the development of functional guest–host systems based on porous architectures.

关键词： heterometallic zeolitic imidazolate frameworks nanopore intrusion hydrogen bonds

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Piezoelectric-enhanced n-TiO2/BaTiO3/p-TiO2 heterojunction for highly efficient photoelectrocatalysis

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green energy & Environment 2024年第9期9卷 1466-1476页

作者： Minhua Ai Zihang Peng Xidi Li Faryal Idrees Xiangwen Zhang Ji-Jun Zou Lun Pan Key Laboratory for green chemical Technology of the Ministry of Education School of Chemical Engineering and Technology Tianjin University Collaborative Innovative center of chemical Science and engineering (Tianjin) Haihe Laboratory of Sustainable chemical Transformations department of Physics University of the Punjab Quaid-e-Azam Campus

Charge separation is critical for achieving efficient solar-to-hydrogen conversion,whereas piezoelectric-enhanced photoelectrochemical（PEC） systems can effectively modulate band bending and charge ***,we design an n-Ti O2/Ba Ti O3/p-Ti O2（TBTm） heterojunction in which the piezoelectric Ba Ti O3layer is sandwiched between n-Ti O2and p-Ti *** built-in electric field of TBTm can provide a strong driving force to accelerate carrier separation and prolong carrier ***,the TBT3 achieves a prominent photocurrent density,as high as 2.13 m A cm-2at 1.23 V versus reversible hydrogen electrode （RHE）,which is 2.4-and 1.5-times higher than Ti O2and Ti O2–Ba Ti O3heterojunction,*** by mechanical deformation,the induced dipole polarization can further regulate built-in electric fields,and the piezoelectric photocurrent density of TBT3-800 is 2.84 times higher than Ti O2at 1.23 V *** due to the construction of *** work provides a piezoelectric polarization strategy for modulating the built-in electric field of heterojunction for PEC system.

关键词： Photoelectrochemical Piezoelectric polarization Heterojunction Charge separation

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A MOF/poly(thioctic acid)composite for enhanced gold extraction from water matrices

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Nano Research 2024年第1期17卷 382-389页

作者： Ruiqing Li Sen Yan Tianwei Xue Rongxing Qiu Yin Li Wenli Hao Guangkuo Xu Yanliang Wang Yanzhen Hong Yuzhong Su Hongtao Wang Shuliang Yang Li Peng Jun Li College of Chemistry and chemical engineering Xiamen UniversityXiamen 361005China department of chemical Physics University of Science and Technology of ChinaHefei 230026China College of energy Xiamen UniversityXiamen 361005China National engineering Laboratory for green chemical Productions of Alcohols Ethers and EstersXiamen UniversityXiamen 361005China Collaborative Innovation center of Chemistry for energy Materials Xiamen UniversityXiamen 361005China

With the fast generation of electronic waste(e-waste)and the increasing depletion of metal resources,“urban mining”that can selectively recover gold from secondary resources has attracted great *** of materials with high extraction capacity and satisfying selectivity in complex aqueous-based matrices still remains ***,a novel metal-organic framework/polymer composite(Fe-BTC/poly(thioctic acid),denoted as Fe-BTC/pTA)has been newly synthesized and applied for selective gold recovery in different matrices(river water,seawater,and leaching solution of e-waste).Benefiting from the high specific surface area and suitable pore sizes as well as the rational design of active sites,the composite exhibits high adsorption capacity(920 mg/g),high removal efficiency(>99%),fast kinetics(below 0.1 ppb within 10 min),and good applicability in complex matrices,which are better than those of most reported sulfur-containing ***-state metallic gold with high purity can be effectively enriched due to the high recyclability and long-term stability of the *** material after adsorption can be further applied as a heterogeneous catalyst for water remediation due to the in situ generated gold nanoparticles by the redox reaction between Au(III)ions and the S-containing groups in the composites.

关键词： metal-organic frameworks(MOFs) poly(thioctic acid)(pTA) polymer composites gold recovery urban mining

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Solvation Effects on the Dielectric Constant of 1 M LiPF6 in Ethylene Carbonate:Ethyl Methyl Carbonate 3:7

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energy & Environmental Materials 2024年第1期7卷 257-260页

作者： Julian Self Nathan T.Hahn Kristin A.Persson department of chemical engineering Polytechnique Montreal department of Materials Science and engineering University of California energy Technologies Area Lawrence Berkeley National Laboratory Material Physical and Chemical Sciences Center Sandia National Laboratories

We report the dielectric constant of 1 M LiPF6in EC:EMC 3:7 w/w（ethylene carbonate/ethyl methyl carbonate） in addition to neat EC:EMC 3:7 w/*** three Debye relaxations,the static permittivity value,or dielectric con... 详细信息

关键词： batteries dielectric relaxation spectroscopy electrolytes

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Deep decalcification of factory-provided freezing acidolysis solution to achieveα-high-strength gypsum

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Chinese Journal of chemical engineering 2024年第5期69卷 143-151页

作者： Wencai Ye Yulu Li Yonggang Dong Lin Yang Yun Yi Jianxin Cao School of Chemistry and chemical engineering Guizhou UniversityGuiyang 550025China engineering Research center of Efficient Utilization for Industrial Waste Guizhou UniversityGuiyang 550025China Key Laboratory of Guizhou Province for green chemical Industry and Clean energy Technology Guizhou UniversityGuiyang 550025China

The freezing acidolysis solution of the nitric acid-phosphate fertilizer process has a high calcium content,which makes it difficult to produce fine phosphate and high water-soluble phosphate fertilizer ***,based on the potential crystallization principle of calcium sulfate in NH_(4)NO_(3)-H_(3)PO_(4)-H_(2)O,the deep decalcification(*** removal)technology to achieveα-high-strength gypsum originated from freezing acidolysis-solutions has been firstly proposed and ***,calcium can be removed from the factory-provided freezing acidolysis-solution by neutralizing it with ammonia,followed by the addition of ammonium sulfate *** a result,the formation of calcium sulfate in the reaction system undergoes the nucleation and growth of CaSO_(4)·2H_(2)O(DH),as well as its dissolution and crystallization into short columnarα-CaSO_(4)·0.5H_(2)O(α-HH).Remarkably,with the molar ratio of SO_(4)^(2-)/Ca^(2+)at 1.8,the degree of neutralization(NH_(3)/HNO_(3) molar ratio)at 1.7,the reaction temperature of 94℃,and the reaction time of 300 min,the decalcification rate can reach 86.89%,of which the high-strengthα-CaSO_(4)·0.5H_(2)O(α-HH)will be ***,the deep decalcification product meets the standards for the production of fine phosphates and highly water-soluble phosphate ***,the 2 h flexural strength ofα-HH is 5.3 MPa and the dry compressive strength is 36.8 MPa,which is up to the standard of commercialα-HH.

关键词： Nitrophosphate Ammonia neutralization Deep decalcification High-strengthα-hemihydrate gypsum Controlled crystallization at atmospheric pressure

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Optimizing 3d spin polarization of CoOOH by in situ Mo doping for efficient oxygen evolution reaction

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Carbon energy 2024年第1期6卷 236-244页

作者： Zhichao Jia Yang Yuan Yanxing Zhang Xiang Lyu Chenhong Liu Xiaoli Yang Zhengyu Bai Haijiang Wang Lin Yang Key Laboratory of green chemical Media and Reactions School of Chemistry and Chemical EngineeringCollaborative Innovation Center of Henan Province for Green Manufacturing of Fine ChemicalsMinistry of EducationHenan Normal UniversityXinxiangHenanChina School of Physics Henan Normal UniversityXinxiangHenanChina Oak Ridge National Laboratory Electrification and Energy Infrastructures DivisionOak RidgeTennesseeUSA department of Mechanical and energy engineering Key Laboratory of Energy Conversion and Storage TechnologiesSouthern University of Science and TechnologyShenzhenGuangdongChina

Transition-metal oxyhydroxides are attractive catalysts for oxygen evolution reactions(OERs).Further studies for developing transition-metal oxyhydroxide catalysts and understanding their catalytic mechanisms will benefit their quick transition to the next ***,Mo-doped CoOOH was designed as a high-performance model electrocatalyst with durability for 20 h at 10 mAcm−***,it had an overpotential of 260 mV(glassy carbon)or 215 mV(nickel foam),which was 78 mV lower than that of IrO_(2)(338 mV).In situ,Raman spectroscopy revealed the transformation process of *** using the density functional theory showed that during OER,doped Mo increased the spin-up density of states and shrank the spin-down bandgap of the 3d orbits in the reconstructed CoOOH under the electrochemical activation process,which simultaneously optimized the adsorption and electron conduction of oxygen-related intermediates on Co sites and lowered the OER *** research provides new insights into the methodical planning of the creation of transition-metal oxyhydroxide OER catalysts.

关键词： electrocatalyst in situ Raman Mo-doped CoOOH oxygen evolution reaction

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Confinement of ionomer for electrocatalytic CO2 reduction reaction via efficient mass transfer pathways

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National Science Review 2024年第2期11卷 168-176页

作者： Xiaowei Du Peng Zhang Gong Zhang Hui Gao Lili Zhang Mengmeng Zhang Tuo Wang Jinlong Gong School of chemical engineering and Technology Key Laboratory for Green Chemical Technology of the Ministry of Education Tianjin University Collaborative Innovation center of chemical Science and engineering(Tianjin) National Industry-Education Platform of energy Storage Tianjin University Joint School of the National University of Singapore and Tianjin University International Campus of Tianjin University Haihe Laboratory of Sustainable chemical Transformations

Gas diffusion electrodes（GDEs） mediate the transport of reactants, products and electrons for the electrocatalytic CO2reduction reaction（CO2RR） in membrane electrode assemblies. The random distribution of ionomer, added by the traditional physical mixing method, in the catalyst layer of GDEs affects the transport of ions and CO2. Such a phenomenon results in elevated cell voltage and decaying selectivity at high current densities. This paper describes a pre-confinement method to construct GDEs with homogeneously distributed ionomer, which enhances mass transfer locally at the active centers. The optimized GDE exhibited comparatively low cell voltages and high CO Faradaic efficiencies（FE > 90%） at a wide range of current densities. It can also operate stably for over 220 h with the cell voltage staying almost unchanged. This good performance can be preserved even with diluted CO2feeds, which is essential for pursuing a high single-pass conversion rate. This study provides a new approach to building efficient mass transfer pathways for ions and reactants in GDEs to promote the electrocatalytic CO2RR for practical applications.

关键词： CO2 electroreduction gas diffusion electrode mass transfer ionomer Ag catalyst

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Prediction of Ground State Configurations and Electrochemical Properties of Li_(3)InCl_(6) Doped with F, Br, and Ga

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Chinese Physics Letters 2024年第5期41卷 171-176页

作者：鲁征宇陈乐添胡绪陈素雅张旭周震 department of Materials Science and engineering Nankai UniversityTianjin 300350China Interdisciplinary Research center for Sustainable energy Science and engineering School of Chemical EngineeringZhengzhou UniversityZhengzhou 450001China

Compared with conventional solid-state electrolytes, halide solid-state electrolytes have several advantages such as a wider electrochemical window, better compatibility with oxide cathode materials, improved air stability,and easier preparation conditions making them conductive to industrial production. We concentrate on a typical halide solid-state electrolyte, Li_(3)InCl_(6), predict the most stable structure after doping with Br, F, and Ga by using the Alloy Theoretic Automated Toolkit based on first-principles calculations, and verify the accuracy of the prediction model. To investigate the potential of three equivalently doped ground state configurations of Li_(3)InCl_(6) as solid-state electrolytes for all-solid-state lithium-ion batteries, their specific properties such as crystal structure,band gap, convex packing energy, electrochemical stability window, and lithium-ion conductivity are computationally analyzed using first-principles calculations. After a comprehensive evaluation, it is determined that the F-doped ground state configuration Li_(3)InCl_(2.5)F_(3.5) exhibits better thermal stability, wider electrochemical stability window, and better lithium ion conductivity(1.80 m S·cm^(-1) at room temperature). Therefore, Li_(3)InCl_(2.5)F_(3.5) has the potential to be used in the field of all-solid-state lithium-ion batteries as a new type of halide electrolyte.

关键词： lithium stability electrolyte

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A zincophilic molecular brush for a dendrite-free,corrosionresistant,zinc metal anode with a long life cycle

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Nano Research 2024年第1期17卷 390-396页

作者： Penggao Liu Jia Guo Xinyue Chen Ting Wang Yanping Huang Shasha Gao Tao Wang Dongling Wu Kaiyu Liu State Key Laboratory of Chemistry and Utilization of Carbon based energy Resources College of ChemistryXinjiang UniversityUrumqi 830017China Hunan Provincial Key Laboratory of chemical Power Sources College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China Key Laboratory of New Low-carbon green chemical Technology School of Chemistry and Chemical EngineeringEducation Department of Guangxi Zhuang Autonomous RegionGuangxi UniversityNanning 530004China Key Laboratory of Microelectronics and energy of Henan Province Department of Physics and Electronic EngineeringXinyang Normal UniversityXinyang 464000China Interdisciplinary Research center for Sustainable energy Science and engineering(IRC4SE2) School of Chemical EngineeringZhengzhou UniversityZhengzhou 450001China

Zinc-based aqueous rechargeable batteries have attracted extensive attention due to their low cost,safety,and environmental ***,dendrite growth and hydrogen evolution of Zn anodes limit their large-scale application.A new strategy to produce a polyacrylamide/reduced graphene oxide(PAM@rGO)molecular nanobrush coating and control Zn electrolyte interface engineering is proposed for use in highly reversible Zn plating/*** evolution is inhibited,and Zn deposition is consolidated using the rich zincophilic functional groups of the branched polyacrylamide chain and the high conductivity of *** to the synergistic effects of corrosion resistance and dendrite-free growth,PAM@rGO/Zn provides prolonged and reversible Zn plating/*** functional theory(DFT)calculations expand on homogenized *** PAM@rGO/Zn||activated carbon(AC)capacitor exhibits long cyclic stability,fast ion transfer,and minimal interfacial *** study provides experimental and theoretical bases for the structural design of Zn anode.

关键词： zincophilic nanobrush polyacrylamide/reduced graphene oxide(PAM@rGO)/Zn surface modification Zn based energy storage

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Stable operation of highly loaded pure Si-Fe anode under ambient pressure via carboxy silane-directed robust solid electrolyte interphase

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Journal of energy Chemistry 2024年第7期94卷 568-576页

作者： Guntae Lim Dong Guk Kang Hyeon Gyu Lee Yen Hai Thi Tran Kihun An Junghyun Choi Kwang Chul Roh Do Youb Kim Seung-Wan Song department of chemical engineering&Applied Chemistry Chungnam National University Daejeon 34134Republic of Korea energy Storage Materials center Korea Institute of Ceramic Engineering&TechnologyJinju 52851Republic of Korea Advanced energy Materials Research center Korea Research Institute of Chemical TechnologyDaejeon 34114Republic of Korea

Incorporation of higher content Si anode material beyond 5 wt% to Li-ion batteries(LIBs)is challenging,owing to large volume change,swelling,and solid electrolyte interphase(SEI)instability ***,a strategy of diacetoxydimethylsilane(DAMS)additive-directed SEI stabilization is proposed for a stable operation of Si-0.33FeSi_(2)(named as Si-Fe)anode without graphite,which provides siloxane inorganics and organics enrichment that compensate insufficient passivation of fluoroethylene carbonate(FEC)additive and reduce a dependence on *** stable cycling performance of highly loaded(3.5 mA h cm^(-2))pure Si-Fe anode is achieved with 2 wt%DAMS combined with 9 wt%FEC additives under ambient pressure,yielding high capacity 1270 mA h g^(-1)at 0.5 C and significantly improved capacity retention of 81% after 100 cycles,whereas short circuit and rapid capacity fade occur with FEC only ***-directed robust SEI layer dramatically suppresses swelling and particles crossover through separator,and therefore prevents short circuit,demonstrating a possible operation of pure Si or Sidominant anodes in the next-generation high-energy-density and safe LIBs.

关键词： High-energy Li-ion battery Pure Si-Fe anode without graphite Silane additive SEI layer Suppressed swelling

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