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Two-dimensional C_(2)N-based single-atom catalyst with complex microenvironment for enhanced electrochemical nitrogen reduction:A descriptor-based design

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Journal of Energy Chemistry 2024年第10期97卷 110-119,I0003页

作者： Enduo Dai Wei An Ruixian Guo Xugen Shi Yunyi Li Yibo Wang Mingming Liu college of Chemistry and chemical engineering.Shanghai University of engineering Science Shanghai 201620China

The catalytic descriptor with operational feasibility is highly desired towards rational design of high-performance catalyst especially the electrode/electrolyte solution interface working under mild ***,we demonstrate that the descriptorΩparameterized by readily accessible intrinsic properties of metal center and coordination is highly operational and efficient in rational design of single-atom catalyst(SAC)for driving electrochemical nitrogen reduction(NRR).Using twodimensional metal(M)-B_(x)P_(y)S_(z)N_m@C_(2)N as prototype SAC models,we reveal that^(*)N_(2)+(H~++e~-)→^(*)N_(2)H acts predominantly as the potential-limiting step(PLS)of NRR on M-B_(2)P_(2)S_(2)@C_(2)N and M-B_(1)P_(1)S_(1)N_(3)@C_(2)N regardless of the distinction in coordination *** the 28 screened M active sites,withΩvalues close to the optimal 4,M-B_(2)P_(2)S_(2)@C_(2)N(M=V(Ω=3.53),Mo(Ω=5.12),and W(Ω=3.92))and M-B_(1)P_(1)S_(1)N_(3)@C_(2)N(M=V(Ω=3.00),Mo(Ω=4.34),and W(Ω=3.32))yield the lowered limiting potential(U_(L))as-0.45,-0.54.-0.36,-0.58,-0.25,and-0.24 V,respectively,thus making them the promising NRR *** importantly,these SACs are located around the top of volcano-shape plot of U_(L) versusΩ,re-validatingΩas an effective descriptor for accurately predicting the high-activity NRR SACs even with complex *** study unravels the relationship between active-site structure and NRR performance via the descriptorΩ,which can be applied to other important sustainable electrocatalytic reactions involving activation of small molecules viaσ-donation andπ^(*)-backdonation mechanism.

关键词： Electrocatalysis N_(2) reduction Single-atom catalyst Descriptor DFT

All-fluorinated electrolyte for non-flammable batteries with ultra-high specific capacity at 4.7 V

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Green Energy & Environment 2024年第10期9卷 1601-1609页

作者： Zhe Wang Zhuo Li Jialong Fu Sheng Zheng Rui Yu Xiaoyan Zhou Guanjie He Xin Guo State Key Laboratory of material Processing and Die&Mould Technology Laboratory of Solid State IonicsSchool of Materials Science and EngineeringHuazhong University of Science and Technology Electrochemical Innovation Lab Department of Chemical EngineeringUniversity College London

Li metal batteries （LMBs） with Li Ni0.8Mn0.1Co0.1O2（NMC811） cathodes could release a specific energy of >500 Wh kg-1by increasing the charge ***,high-nickel cathodes working at high voltages accelerate degradations in bulk and at interfaces,thus significantly degrading the cycling lifespan and decreasing the specific ***,we rationally design an all-fluorinated electrolyte with addictive tri（2,2,2-trifluoroethyl） borate （TFEB）,based on 3,3,3-fluoroethylmethylcarbonate （FEMC） and fluoroethylene carbonate （FEC）,which enables stable cycling of high nickel cathode (Li Ni0.8Co0.1Mn0.1O2,NMC811) under a cut-off voltage of 4.7 V in Li metal *** electrolyte not only shows the fire-extinguishing properties,but also inhibits the transition metal dissolution,the gas production,side reactions on the cathode ***,the NMC811||Li cell demonstrates excellent performance by using limited Li and high-loading cathode,delivering a specific capacity>220 m A h g-1,an average Coulombic efficiency >99.6% and capacity retention >99.7% over 100 cycles.

关键词： Fluorinated electrolyte Li metal batteries Solid electrolyte interphase Cathode electrolyte interphase Coulombic efficiency

Mechanism of interfacial effects in sodium-ion storage devices

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Nano Research 2024年第3期17卷 1313-1326页

作者： Yifan Wei Lingxing Zan Huicong Xia Wenfu Yan Jia-Nan Zhang college of materials Science and engineering Zhengzhou UniversityZhengzhou 450001China Key Laboratory of Advanced Energy Catalytic and Functional material Preparation of Zhengzhou City Zhengzhou 450001China Key Laboratory of chemical Reaction engineering of Shaanxi Province College of Chemistry&Chemical EngineeringYan’an UniversityYan’an 716000China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry and college of Chemistry Jilin UniversityChangchun 130012China

Rechargeable sodium-ion batteries(SIBs)are considered as the next-generation secondary *** performance of SIB is determined by the behavior of its electrode surface and the electrode–electrolyte interface during charging and ***,the characteristics of these surfaces and interfaces should be analyzed to realize large-scale energy storage systems with high energy density and long-cycle *** various studies have investigated the properties of electrode materials,few studies have focused on the construction of stable and efficient SIB interfaces,and even fewer have explored the mechanisms of interfacial effects;however,the strategies of regulating interfacial effects are yet to be completely ***,the results obtained thus far are insufficient to draw systematic *** present study reviews the literature on the mechanism of interfacial effects in Na+storage *** interfaces in a sodium-ion storage device include a heterogeneous interface between electrode materials,a solid electrolyte interphase,and a cathode electrolyte *** interfacial effects during the intercalation,transformation,and alloy reactions and the resulting overall battery performance were theoretically *** this review,we aim to provide a theoretical basis for optimizing the structures of electrode surface and electrode–electrolyte interface to optimize the performance of *** addition,the challenges of investigating interfacial effects and several possible helpful methods and opportunities for studying the mechanisms of interfacial effects in SIBs will be presented.

关键词： sodium-ion storage interfacial effects solid electrolyte interphase cathode electrolyte interphase

Thermoregulatory molecular sieving in crystals

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Science China materials 2024年第10期67卷 3419-3420页

作者： Guozhen Liu Wanqin Jin Gongping Liu State Key Laboratory of materials-Oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211800China

Sub-nanometer channels for the selective recognition of the components in chemical mixtures from others play a crucial role in the adsorption and membrane separation[1].It remains a grand challenge to separate small m... 详细信息

关键词： structure. molecular separation

Research progress on simulation of multiscale mass transfer processes in gas-solid system by computational mass transfer

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Particuology 2024年第7期90卷 478-492页

作者： Xu Li Yaohui Wang Leifu Li Runye Zhang Hailun Ren Wenbin Li Zhongli Tang Donghui Zhang The Research Center of chemical engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China The Department of chemical engineering Tianjin Renai CollegeTianjin 301636China Collaborative Innovation Center of chemical Science and engineering(Tianjin) School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Particle-fluid system is one of the most popular systems in chemical *** to complex interface structure and high-velocity turbulence,the momentum and mass transfer exhibit nonlinear characteristics,which pose a great challenge for further study and *** solve this problem,computational mass transfer(CMT)emerged and has been proved to be effective in deeply exploring the mass transfer behavior of particle-fluid ***,this paper reviews recent gas-solid numerical studies of turbulence issues from empirical to theoretical,then discusses interphase mass transfer rate models and the interfacial interaction ***,the present study particularly reviews researches on mass transfer process of fixed and fluidized regime by CMT,providing reliable analysis of turbulent anisotropy diffusivity as well as multiscale structure and presenting theoretical instruction for the industrial optimization of mass transfer processes in chemical engineering.

关键词： Fixed bed Fluidized bed Computational mass transfer Turbulent mass diffusion Multiscale Anisotropy

Investigation into the Methodology and Implementation of Life Cycle engineering under China’s Carbon Reduction Target in the Process Industry

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engineering 2024年第9期40卷 87-99页

作者： Mingyang Li Feng Gao Zuoren Nie Boxue Sun Yu Liu Xianzheng Gong National engineering Laboratory for Industrial Big-data Application Technology College of Material Science and EngineeringBeijing University of TechnologyBeijing 100124China

The industrial sector is the primary source of carbon emissions in *** pursuit of meeting its carbon reduction targets,China aims to promote resource consumption sustainability,reduce energy consumption,and achieve carbon neutrality within its processing *** effective strategy to promote energy savings and carbon reduction throughout the life cycle of materials is by applying life cycle engineering *** strategy aims to attain an optimal solution for material performance,resource consumption,and environmental *** this study,five types of technologies were considered:raw material replacement,process reengineering,fuel replacement,energy recycling and reutilization,and material recycling and *** meaning,methodology,and development status of life cycle engineering technology abroad and domestically are discussed in detail.A multidimensional analysis of ecological design was conducted from the perspectives of resource and energy consumption,carbon emissions,product performance,and recycling of secondary resources in a manufacturing *** coupled with an integrated method to analyze carbon emissions in the entire life cycle of a material process industry was applied to the nonferrous industry,as an *** results provide effective ideas and solutions for achieving low or zero carbon emission production in the Chinese industry as recycled aluminum and primary aluminum based on advanced technologies had reduced resource consumption and emissions as compared to primary aluminum production.

关键词： Carbon neutrality Life cycle engineering Process Industry Carbon reduction technology Eco-design

Preparation and properties of poly(ethylene glycol)-bpoly( 3-acrylamidophenylboronic acid) glucose responsive particles and their hyaluronic acid-based microneedle patches

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Journal of Zhejiang University-Science A(Applied Physics & engineering) 2024年第5期25卷 395-410页

作者： Yichuan HONG Haojie YU Li WANG Xiang CHEN Di SHEN Yu WANG Shuning REN Yudi HUANG Jian YANG State Key Laboratory of chemical engineering College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310058China Zhejiang-Russia Joint Laboratory of Photo-Electro-Magnetic Functional materials College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310058China

To overcome the pain and risk of hypoglycemia in insulin administration,glucose-responsive microneedles have been developed by researchers,which could release insulin according to the blood glucose *** designed a kind of particles by a reversible addition-fragmentation chain transfer(RAFT)method containing a phenylboronic acid group as the sensor of glucose and carrier of ***(ethylene glycol)(PEG)-2-(dodecylthio(thiocarbonyl)thio)-2-methylpropionic acid(DDMAT)was synthesized as a macromolecular RAFT agent,which was then reacted with 3-acrylamidophenylboronic acid(AAPBA)to synthesize the block copolymer ***-responsive particles loaded with insulin were prepared by self-assembly based on hydrophilic-hydrophobic *** patches loaded with glucose-responsive particles were prepared using hyaluronic acid as the *** insulin release behavior of the particles in glucose solutions of 0,100,and 400 mg/dL showed significant glucose responsiveness and good *** results of blood glucose control experiments in rats indicate that a single microneedle patch can effectively maintain normal blood glucose for over 7 h.

关键词： Diabetes Hyaluronic acid Phenylboronic acid(PBA) Glucose responsive hydrogel Microneedles

Controlling reversible complexation-mediated polymerization(RCMP)via deep eutectic solvents:fast kinetics,narrow molecular weight distribution and mechanistic insights

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Science China Chemistry 2024年第8期67卷 2728-2736页

作者： Xin Fu Zhen Lu Shen Li Zheng-Hong Luo Lin-Xi Hou Department of materials-Oriented chemical engineering College of Chemical EngineeringFuzhou UniversityFuzhou 350116China Department of chemical engineering School of Chemistry and Chemical EngineeringState Key Laboratory of Metal Matrix CompositesShanghai Jiao Tong UniversityShanghai 200030China chemical engineering Zhicheng College of Fuzhou UniversityFuzhou 350116China Qingyuan Innovation Laboratory Quanzhou 362801China

The exploitation of new green polymerization avenues for the effective synthesis of polymers by reversible-deactivation radical polymerization plays a critical role in pursuing the development of polymeric *** this work,serials of deep eutectic solvents(DES)with intermolecular-hydrogen-bonding interaction were constructed as catalysts and medium for actuating reversible complexation-mediated polymerization(RCMP)for the first time,yielding methacrylate polymers with high monomer conversion and narrow dispersion molecular weight in both water and oil *** mechanism and elementary reaction of RCMP were explored deeply,revealing that the complexation of initiator with DES to generate radicals was a ratecontrolling step and intermolecular-hydrogen-bond was primary factor to influence polymerization ***,the insights of density functional theory calculations revealed that negative electrostatic potential ensured nucleophilic *** investigation demonstrated the considerable potential of DES for RCMP,which is anticipated for other polymerization applications as a novel medium mode.

关键词： deep eutectic solvent reversible complexation-mediated polymerization intermolecular hydrogen bonding density functional theory elementary reaction steps

Rational design of practical layered transition metal oxide cathode materials for sodium-ion batteries

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Frontiers of chemical Science and engineering 2024年第7期18卷 121-140页

作者： Yan Wang Ning Ding Rui Zhang Guanhua Jin Dan Sun Yougen Tang Haiyan Wang Hunan Provincial Key Laboratory of chemical Power Sources College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China college of Energy and chemical engineering Xinjiang Institute of TechnologyAksu Prefecture 843100China

Sodium-ion batteries (SIBs), which serve as alternatives or supplements to lithium-ion batteries, have been developed rapidly in recent years. Designing advanced high-performance layered NaxTMO_(2) cathode materials is beneficial for accelerating the commercialization of SIBs. Herein, the recent research progress on scalable synthesis methods, challenges on the path to commercialization and practical material design strategies for layered NaxTMO_(2) cathode materials is summarized. Co-precipitation method and solid-phase method are commonly used to synthesize NaxTMO_(2) on mass production and show their own advantages and disadvantages in terms of manufacturing cost, operative difficulty, sample quality and so on. To overcome drawbacks of layered NaxTMO_(2) cathode materials and meet the requirements for practical application, a detailed and deep understanding of development trends of layered NaxTMO_(2) cathode materials is also provided, including high specific energy materials, high-entropy oxides, single crystal materials, wide operation temperature materials and high air stability materials. This work can provide useful guidance in developing practical layered NaxTMO_(2) cathode materials for commercial SIBs.

关键词： sodium-ion batteries layered oxide industrialization development prospect