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Catalyst design and structure control for photocatalytic refineries of cellulosic biomass to fuels and chemicals

Journal of energy Chemistry 2024年第7期94卷 102-127页

作者： Lulu Sun Nengchao Luo state key laboratory of catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina

Lignocellulosic biomass is the largest renewable hydrocarbon resource on *** cellulose,one of the major components of lignocellulose,powered by solar energy is a promising way of providing lowcarbon-footprint energy chemicals such as H_(2),HCOOH,CO,and transportation ***-of-the-art biorefineries target the full use of biomass feedstocks as they have a maximum collection radius of 75-100 km,requesting efficient and selective photocatalysts that significantly influence the outcome of photocatalytic ***-performed photocatalysts can harvest a broad solar spectrum and are active in breaking the chemical bonds of cellulose,decreasing the capital investments of ***,photocatalysts should control the selectivity of cellulose conversion,originating target products to level down separation *** separation in photocatalysts and interfacial charge transfer between photocatalysts and cellulose affect the activity and selectivity of cellulose refineries to H2 and carbonaceous *** account for the challenges above,this review summarizes photocatalysts for the refineries of cellulose and downstream platform molecules based on the types of products,with the structure features of different types of photocatalysts discussed in relation to the targets of either improving the activity or product *** addition,this review also sheds light on the methods for designing and regulating photocatalyst structures to facilitate photocatalytic refineries of cellulose and platform molecules,meanwhile summarizing proposed future research challenges and opportunities for designing efficient photocatalysts.

关键词： Photocatalysts Biorefineries Cellulose Fuels Hydrogen

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High-Voltage and Fast-Charging Lithium Cobalt Oxide Cathodes: From key Challenges and Strategies to Future Perspectives

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Engineering 2024年第6期37卷 105-127页

作者： Gongrui Wang Zhihong Bi Anping Zhang Pratteek Das Hu Lin Zhong-Shuai Wu state key laboratory of catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China dalian national laboratory for clean energy Chinese Academy of SciencesDalian 116023China

Lithium-ion batteries(LIBs)with the“double-high”characteristics of high energy density and high power density are in urgent demand for facilitating the development of advanced portable ***,the lithium ion(Li+)-storage performance of the most commercialized lithium cobalt oxide(LiCoO_(2),LCO)cathodes is still far from satisfactory in terms of high-voltage and fast-charging capabilities for reaching the double-high ***,we systematically summarize and discuss high-voltage and fast-charging LCO cathodes,covering in depth the key fundamental challenges,latest advancements in modification strategies,and future perspectives in this *** and elaborated discussions are first presented on key fundamental challenges related to structural degradation,interfacial instability,the inhomogeneity reactions,and sluggish interfacial *** provide an instructive summary of deep insights into promising modification strategies and underlying mechanisms,categorized into element doping(Li-site,cobalt-/oxygen-site,and multi-site doping)for improved Li+diffusivity and bulkstructure stability;surface coating(dielectrics,ionic/electronic conductors,and their combination)for surface stability and conductivity;nanosizing;combinations of these strategies;and other strategies(i.e.,optimization of the electrolyte,binder,tortuosity of electrodes,charging protocols,and prelithiation methods).Finally,forward-looking perspectives and promising directions are sketched out and insightfully elucidated,providing constructive suggestions and instructions for designing and realizing high-voltage and fast-charging LCO cathodes for next-generation double-high LIBs.

关键词： Lithium cobalt oxide High energy/power density Fast-charging High-voltage Lithium-ion battery

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Hybrid ion/electron interfacial regulation stabilizes the cobalt/oxygen redox of ultrahigh-voltage lithium cobalt oxide for fast-charging cyclability

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Science Bulletin 2024年第13期69卷 2071-2079页

作者： Zhihong Bi Anping Zhang Gongrui Wang Cong Dong Pratteek Das Xiaoyu Shi Zhong-Shuai Wu state key laboratory of catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China dalian national laboratory of clean energy Chinese Academy of SciencesDalian 116023China

High-voltage and fast-charging LiCoO_(2)(LCO)is key to high-energy/power-density Li-ion ***,unstable surface structure and unfavorable electronic/ionic conductivity severely hinder its high-voltage fast-charging ***,we construct a Li/Na-B-Mg-Si-O-F-rich mixed ion/electron interface network on the 4.65 V LCO electrode to enhance its rate capability and long-term cycling ***,the resulting artificial hybrid conductive network enhances the reversible conversion of Co^(3+)/^(4+)/O_(2)/nredox by the interfacial ion–electron cooperation and suppresses interface side reactions,inducing an ultrathin yet compact cathode electrolyte ***,the derived near-surface Na+/Mg2+/Si^(4+)-pillared local intercalation structure greatly promotes the Li^(+)diffusion around the 4.55 V phase transition and stabilizes the cathode ***,excellent 3 C(1 C=274 mA g1)fast charging performance is demonstrated with 73.8%capacity retention over 1000 *** findings shed new insights to the fundamental mechanism of interfacial ion/electron synergy in stabilizing and enhancing fast-charging cathode materials.

关键词： High-voltage Fast-charging LiCoO_(2) Interfacial ion-electron cooperation Local intercalation

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Unleashing the Power of Bio-based Thermotropic Liquid Crystal Modifiers:Toughening and Reinforcing Petroleum-based Epoxy Resin without Compromising Other Properties

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Chinese Journal of Polymer Science 2024年第8期42卷 1093-1102页

作者： Qing-Yun Lu Hong-Wei Gu Jia-Hui Li Qian-Qian Fan Bei-Tao Liu Yan Kou Xi-Gao Jian Zhi-Huan Weng state key laboratory of Fine Chemicals Frontiers Science Center for Smart MaterialsLiaoning Technology Innovation Center of High Performance Resin MaterialsDepartment of Polymer Science&EngineeringDalian University of TechnologyDalian 116024China Thermochemistry laboratory Liaoning Province Key Laboratory of Thermochemistry for Energy and MaterialsDalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

Toughening the petroleum-based epoxy resin blends with bio-based modifiers without compromising their modulus,mechanical strength,and other properties is still a big challenge in view of the *** this study,a bio-based liquid crystal epoxy resin(THMT-E P)with an s-triazine ring structure was utilized to modify a petroleum-based bisphenol A epoxy resin(E51)with 4,4'-diaminodiphenylsulfone(DDS)as a curing agent,and the blended systems were evaluated for their thermal stability,mechanical properties,and flame *** results showed that the impact strength of the blended system initially increased and then decreased with the increase in THMT-EP content,and it reached the a maximum value of 26.5 kJ/m^(2)when the THMT-EP content was 5%,which was 31.2%higher than that of E51/***,the flexural strength,modulus,and glass transition tem perature of the blended system were all simultaneously improved with the addition of *** the same time,the addition of THMT-EP enhanced the flame retardancy of the system by increasing the char yield at 700℃and decreasing the peak heat release rate and total heat release *** work paves the way for a more sustainable improvement in the comprehensive performance of epoxy resin.

关键词： Epoxy resin Toughening Bio-based Thermotropic liquid crystal

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SEI/dead Li-turning capacity loss for high-performance anode-free solid-state lithium batteries

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Journal of energy Chemistry 2024年第9期96卷 145-152页

作者： Qianwen Yin Tianyu Li Hongzhang Zhang Guiming Zhong Xiaofei Yang Xianfeng Li Division of energy Storage Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China key laboratory of Long-Duration and Large-Scale energy Storage Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina laboratory of Advanced Spectro-Electrochemistry and Lithium-Ion Batteries Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina

Anode-free solid-state lithium metal batteries(AF-SSLBs)have the potential to deliver higher energy density and improved safety beyond lithium-metal ***,the unclear mechanism for the fast capacity decay in AF-SSLBs,either determined by dead Li or solid electrolyte interface(SEI),limits the proposal of effective strategies to prolong cycling *** clarify the underlying mechanism,herein,the evolution of SEI and dead Li is quantitatively analyzed by a solid-state nuclear magnetic resonance(ss-NMR)technology in a typical LiPF6-based polymer *** results show that the initial capacity loss is attributed to the formation of SEI,while the dead Li dominates the following capacity loss and the growth rate is 0.141 mA h cm^(−2)cycle−*** reduce the active Li loss,the combination of inorganic-rich SEI and self-healing electrostatic shield effect is proposed to improve the reversibility of Li deposition/dissolution behavior,which reduces the capacity loss rate for the initial SEI and following dead Li generation by 2.3 and 20.1 folds,*** a result,the initial Coulombic efficiency(ICE)and stable CE increase by 15.1%and 15.3%in Li-Cu cells,which guides the rational design of high-performance AF-SSLBs.

关键词： Solid-state lithium batteries Solid-state NMR Anode-free SEI Dead Li

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高电压快充钴酸锂正极——关键挑战、改性策略与未来展望（英文）

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Engineering 2024年第6期 105-127页

作者：王功瑞毕志宏张安萍 Pratteek Das 林虎吴忠帅 state key laboratory of catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences dalian national laboratory for clean energy Chinese Academy of Sciences

Lithium-ion batteries（LIBs） with the ‘‘double-high” characteristics of high energy density and high power density are in urgent demand for facilitating the development of advanced portable electronics. However,the lithium ion（Li+）-storage performance of the most commercialized lithium cobalt oxide（LiCoO2, LCO）cathodes is still far from satisfactory in terms of high-voltage and fast-charging capabilities for reaching the double-high target. Herein, we systematically summarize and discuss high-voltage and fast-charging LCO cathodes, covering in depth the key fundamental challenges, latest advancements in modification strategies, and future perspectives in this field. Comprehensive and elaborated discussions are first presented on key fundamental challenges related to structural degradation, interfacial instability, the inhomogeneity reactions, and sluggish interfacial kinetics. We provide an instructive summary of deep insights into promising modification strategies and underlying mechanisms, categorized into element doping（Li-site, cobalt-/oxygen-site, and multi-site doping） for improved Li+diffusivity and bulkstructure stability; surface coating（dielectrics, ionic/electronic conductors, and their combination） for surface stability and conductivity; nanosizing; combinations of these strategies; and other strategies（i.e., optimization of the electrolyte, binder, tortuosity of electrodes, charging protocols, and prelithiation methods）. Finally, forward-looking perspectives and promising directions are sketched out and insightfully elucidated, providing constructive suggestions and instructions for designing and realizing high-voltage and fast-charging LCO cathodes for next-generation double-high LIBs.

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Application of machine learning in perovskite materials and devices:A review

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Journal of energy Chemistry 2024年第7期94卷 254-272页

作者： Ming Chen Zhenhua Yin Zhicheng Shan Xiaokai Zheng Lei Liu Zhonghua Dai Jun Zhang Shengzhong(Frank)Liu Zhuo Xu School of Electric Power Civil Engineering and ArchitectureCollege of Physics and Electronics EngineeringState Key Laboratory of Quantum Optics and Quantum Optics DevicesShanxiUniversityTaiyuan030006ShanxiChina key laboratory of Applied Surface and Colloid Chemistry National Ministry of EducationShanxi Engineering Lab for Advanced Energy TechnologySchool of Materials Science and EngineeringShaanxi Normal UniversityXi'an 710119ShaanxiChina state key laboratory of catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina

Metal-halide hybrid perovskite materials are excellent candidates for solar cells and photoelectric *** recent years,machine learning(ML)techniques have developed rapidly in many fields and provided ideas for material discovery and *** can be applied to discover new materials quickly and effectively,with significant savings in resources and time compared with traditional experiments and density functional theory(DFT)*** this review,we present the application of ML in per-ovskites and briefly review the recent works in the field of ML-assisted perovskite ***,the advantages of perovskites in solar cells and the merits of ML applied to perovskites are ***,the workflow of ML in perovskite design and some basic ML algorithms are ***,the applications of ML in predicting various properties of perovskite materials and devices are ***,we propose some prospects for the future development of this *** rapid devel-opment of ML technology will largely promote the process of materials science,and ML will become an increasingly popular method for predicting the target properties of materials and devices.

关键词： Machine learning Perovskite Materials design Bandgap engineering Stability Crystal structure

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Mechanism of high Li-ion conductivity in poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network based electrolyte revealed by solid-state NMR

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Journal of energy Chemistry 2024年第6期93卷 377-383,I0010页

作者： Fan Li Tiantian Dong Yi Ji Lixin Liang Kuizhi Chen Huanrui Zhang Guanglei Cui Guangjin Hou state key laboratory of catalysis Dalian National Laboratory for Clean EnergyCollaborative Innovation Center of Chemistry for Energy MaterialsDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China Qingdao Industrial energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101ShandongChina

Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid ***-linked polymers have the potential to further improve the mechanical property without trading off Li-ion *** this study,focusing on a recently developed cross-linked SPE,i.e.,the one based on poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network(PVCN),we used solid-state nuclear magnetic resonance(NMR)techniques to investigate the fundamental interaction between the chain segments and Li ions,as well as the lithium-ion *** utilizing homonuclear/heteronuclear correlation,CP(cross-polarization)kinetics,and spin-lattice relaxation experiments,etc.,we revealed the structural characteristics and their relations to lithium-ion *** is found that the network formation prevents poly(ethylene oxide)chains from crystallization,which could create sufficient space for segmental tumbling and Li-ion co nductio *** such,the mechanical property is greatly improved with even higher Li-ion mobilities compared to the poly(vinylene carbonate)or poly(ethylene oxide)based SPE analogues.

关键词： ssNMR Lithium-ion mobility Cross-link Solid polymer electrolyte

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Incorporation sodium ions into monodisperse lead-free double perovskite Cs_(2)AgBiCl_(6) nanocrystals to improve optical properties

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Chinese Chemical Letters 2024年第3期35卷 549-553页

作者： Song Wang Ying Xie Wenchao Jiang Binghang Liu keying Shi Kai Pan key laboratory of Functional Inorganic Material Chemistry Ministry of EducationHeilongjiang UniversityHarbin 150080China School of Materials Science and Engineering Jiangsu Engineering Laboratory of Light-Electricity-Heat Energy-Converting Materials and ApplicationsChangzhou UniversityChangzhou 213164China state key laboratory of catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

Lead-free double perovskite nanocrystals(NCs)have emerged as a promising candidate in the optical field,owing to their non-toxic,good moist heat and chemical ***,their poor optical properties limited their *** improve the optical properties of lead-free double perovskite NCs,metal ion doping or alloying had been suggested as a promising ***,we prepared monodisperse,uniformly sized,cubic morphology of Cs_(2)AgBiCl_(6)NCs with different Na^(+)incorporation amounts via a simple hot-injection *** Na^(+)incorporation broke the parity-forbidden transition by reducing the inversion symmetry of the electron wave function at the Ag site,which changed the parity of the self-trapped exciton wave function and thus allowed radiative *** a result,the photoluminescence quantum yield(PLQY)of Na^(+)-alloyed Cs_(2)AgBiCl_(6)NCs(12.1%)was higher than that of Cs_(2)AgBiCl_(6)NCs(2.4%),and the exciton lifetime of Na^(+)-alloyed Cs_(2)AgBiCl_(6)NCs increased to 36.98 ns from 17.58 ns for Cs_(2)AgBiCl_(6)*** adjusting the amount of Na^(+)incorporation,the band gap of Cs_(2)AgBiCl_(6)NCs can be significantly tuned from~2.90 eV to~3.50 ***,the temperature-dependent photoluminescence spectra indicated that the Na^(+)-alloyed Cs_(2)AgBiCl_(6)NCs possessed higher longitudinal optical phonon energy and exciton binding energy compared to Cs_(2)AgBiCl_(6)*** suggested that there were strong exciton-phonon interactions during exciton recombination,a reduced probability of non-radiative processes,and excellent thermal *** offers a promising strategy for improving the optical properties of lead-free double perovskite NCs,and have the potential to replace traditional lead halide perovskite NCs in future optoelectronic applications.

关键词： Nanocrystals Alloy Double perovskites Optical properties Exciton binding energy

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Oxidative Dehydrogenation of Propane over Supported Nickel Single-Atom Catalyst

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Chinese Journal of Chemistry 2024年第4期42卷 370-376页

作者： Qian Zhang Xunzhu Jiang Yangyang Li Yuanlong Tan Qike Jiang Xiaoyan Liu Botao Qiao CAS key laboratory of Science and Technology on Applied catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianLiaoning116023 China University of Chinese Academy of Sciences Beijing100049 China dalian national laboratory for clean energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianLiaoning116023 China

Oxidative dehydrogenation of propane has been an ever-growing field for propylene production due to its exothermic properties,of which overoxidation is the major drawback,with CO and even CO_(2) as undesired *** the purpose of getting higher propylene selectivity as well as yield,herein,we report Ni single atoms supported on calcium aluminate as an efficient catalyst candidate for propane oxidative *** from higher valence states of Ni1 species,it shows 2—3 times as much propylene selectivity as that of Ni *** 14.2%C_(3)H_(6) yield with 47.3%propylene selectivity has been achieved on Ni single atom catalyst and a good stability during 20 h test can be obtained as well.

关键词： Oxidative dehydrogenation/Nickel Single-atom catalysts Propane Propylene selectivity

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