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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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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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三维碳基导热网络的设计、进展和挑战（英文）

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新型炭材料(中英文) 2024年

作者：井源刘汉卿周锋戴昉纳吴忠帅材料科学与工程学院中国石油大学(华东) 大连化学物理研究所中国科学院大学

5G时代的到来刺激了密集集成化的大功率电子器件的快速发展。三维导热网络具有较高的导热性和导电性，并且结构可调性强，被认为是提高电子器件性能的可行关键材料。在这篇综述中，我们提供了碳基三维导热网络的关键概述，强调了碳材料... 详细信息

5G时代的到来刺激了密集集成化的大功率电子器件的快速发展。三维导热网络具有较高的导热性和导电性，并且结构可调性强，被认为是提高电子器件性能的可行关键材料。在这篇综述中，我们提供了碳基三维导热网络的关键概述，强调了碳材料之间的制备-结构-性能关系及其在不同场景中的应用。首先，详细讨论了热导率的微观原理，这是指导三维碳材料热导率增强的关键因素。此外，本文还深入研究了利用石墨烯、泡沫碳和碳纳米管等不同碳材料构建三维网络的方法。重点介绍了将二维石墨烯组装成三维石墨烯网络的制备技术及其对导热性能的影响。最后，提出了碳基三维导热网络存在的挑战和未来的发展前景。该综述将为下一代三维碳基导热网络材料的设计和构建提供蓝图。

关键词：碳材料三维网络石墨烯导热率热传输

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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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A hybrid spatial-temporal deep learning prediction model of industrial methanol-to-olefins process

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Frontiers of Chemical Science and Engineering 2024年第4期18卷 73-85页

作者： Jibin Zhou Xue Li Duiping Liu Feng Wang Tao Zhang Mao Ye Zhongmin Liu National Engineering Research Center of Lower-Carbon Catalysis Technology Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Yulin Innovation Institute for Clean Energy Clean Energy Innovation Institute of Chinese Academy of SciencesYulin 719053China Xuelang Industrial Intelligence Technology Co. Ltd.Wuxi 214000China

Methanol-to-olefins,as a promising non-oil pathway for the synthesis of light olefins,has been successfully *** accurate prediction of process variables can yield significant benefits for advanced process control and *** challenge of this task is underscored by the failure of traditional methods in capturing the complex characteristics of industrial processes,such as high nonlinearities,dynamics,and data distribution shift caused by diverse operating *** this paper,we propose a novel hybrid spatial-temporal deep learning prediction model to address these ***,a unique data normalization technique called reversible instance normalization is employed to solve the problem of different data ***,convolutional neural network integrated with the self-attention mechanism are utilized to extract the temporal ***,a multi-graph convolutional network is leveraged to model the spatial ***,the extracted temporal and spatial features are fused as input into a fully connected neural network to complete the ***,the outputs are denormalized to obtain the ultimate *** monitoring results of the dynamic trends of process variables in an actual industrial methanol-to-olefins process demonstrate that our model not only achieves superior prediction performance but also can reveal complex spatial-temporal relationships using the learned attention matrices and adjacency matrices,making the model more ***,this model is deployed onto an end-to-end Industrial Internet Platform,which achieves effective practical results.

关键词： methanol-to-olefins process variables prediction spatial-temporal self-attention mechanism graph convolutional network

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Hierarchically Structured Nb_(2)O_5 Microflowers with Enhanced Capacity and Fast-Charging Capability for Flexible Planar Sodium Ion Micro-Supercapacitors

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Nano-Micro Letters 2024年第4期16卷 97-109页

作者： Jiaxin Ma Jieqiong Qin Shuanghao Zheng Yinghua Fu Liping Chi Yaguang Li Cong Dong Bin Li Feifei Xing Haodong Shi Zhong‑Shuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of Sciences457 Zhongshan RoadDalian 116023People’s Republic of China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001People’s Republic of China College of Science Henan Agricultural UniversityNo.63 Agricultural RoadZhengzhou 450002People’s Republic of China Dalian National Laboratory for Clean Energy Chinese Academy of Sciences457 Zhongshan RoadDalian 116023People’s Republic of China University of Chinese Academy of Sciences 19A Yuquan RoadShijingshan DistrictBeijing 100049People’s Republic of China Hebei Key Lab of Optic‑Electronic Information and Materials The College of Physics Science and TechnologyInstitute of Life Science and Green DevelopmentHebei UniversityBaoding 071002People’s Republic of China

Planar Na ion micro-supercapacitors(NIMSCs) that offer both high energy density and power density are deemed to a promising class of miniaturized power sources for wearable and portable microelectron-ics. Nevertheless, the development of NIMSCs are hugely impeded by the low capacity and sluggish Na ion kinetics in the negative ***, we demonstrate a novel carbon-coated Nb_(2)O_5 microflower with a hierarchical structure composed of vertically intercrossed and porous nanosheets, boosting Na ion storage performance. The unique structural merits, including uniform carbon coating, ultrathin nanosheets and abun-dant pores, endow the Nb_(2)O_5 microflower with highly reversible Na ion storage capacity of 245 mAh g^(-1) at 0.25 C and excellent rate *** from high capacity and fast charging of Nb_(2)O_5 microflower, the planar NIMSCs consisted of Nb_(2)O_5 negative electrode and activated car-bon positive electrode deliver high areal energy density of 60.7 μWh cm^(-2),considerable voltage window of 3.5 V and extraordinary cyclability. Therefore, this work exploits a structural design strategy towards electrode materials for application in NIMSCs, holding great promise for flexible microelectronics.

关键词： Nb_(2)O_5 nanosheets Microflowers Sodium ion micro-supercapacitors Flexibility Energy storage

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Engineering FeOOH/Ni(OH)_(2) heterostructures on Ni_(3)S_(2)surface to enhance seawater splitting

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Rare Metals 2024年第5期43卷 1989-1998页

作者： Chen Yang Ya-Dong Li Li-Juan Cao Xi-Long Wang Han-Pu Liang Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266101China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China Sino-Danish College University of Chinese Academy of SciencesBeijing 100049China

The construction of highly stable and efficient electrocatalysts is desirable for seawater splitting but remains challenging due to the high concentration of Cl-in ***,FeOOH/Ni(OH)_(2)heterostructure supported on Ni_(3)S_(2)-covered nickel foam(Fe–Ni/Ni_(3)S_(2)/NF)was fabricated by hydrothermal and etching methods,as well as anodic oxidation *** electronic structure of FeOOH and Ni(OH)_(2)could be modulated after depositing FeOOH nanoparticles on Ni(OH)_(2)nanosheet,which greatly boosted the catalytic *** the catalyst used as an electrode for oxygen evolution reaction(OER),it needed low overpotentials of 266 and 368 m V to achieve current densities of 100 and 800 m A·cm^(-2),respectively,in 1 mol·L^(-1)KOH+seawater *** can operate continuously at 100 m A·cm^(-2)for 400 h without obvious ***,in situ generated SO_(4)^(2-)from inner Ni_(3)S_(2)during electrolysis process would accumulate on the surface of active sites to form passivation layers to repel Cl^(-),which seemed to be responsible for superior *** study not only synthesizes an OER catalyst for highly selective and stable seawater splitting,but also gives a novel approach for industrial hydrogen production.

关键词： Anodic oxidation Heterostructure Oxygen evolution reaction Seawater splitting

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Regulating surface electron structure of PtNi nanoalloy via boron doping for high‐current‐density Li‐O2 batteries with low overpotential and long‐life cyclability

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SmartMat 2024年第1期5卷 110-120页

作者： Yajun Ding Yuanchao Huang Yuejiao Li Tao Zhang Zhong‐Shuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianChina State Key Laboratory of Silicon Materials and School of Materials Science and Engineering Zhejiang UniversityHangzhouChina Institute of Advanced Semiconductors Hangzhou Innovation CenterZhejiang UniversityHangzhouChina University of Chinese Academy of Sciences BeijingChina State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghaiChina Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalianChina

The realization of high‐efficiency,reversible,stable,and safe Li‐O2 batteries is severely hindered by the large overpotential and side reactions,especially at high rate ***,rational design of cathode catalysts with high activity and stability is crucial to overcome the terrible issues at high current ***,we report a surface engineering strategy to adjust the surface electron structure of boron(B)‐doped PtNi nanoalloy on carbon nanotubes(PtNiB@CNTs)as an efficient bifunctional cathodic catalyst for high‐rate and long‐life Li‐O2 ***,the Li‐O2 batteries assembled with as‐prepared PtNiB@CNT catalyst exhibit ultrahigh discharge capacity of 20510 mA·h/g and extremely low overpotential of 0.48 V at a high current density of 1000 mA/g,both of which outperform the most reported Pt‐based catalysts ***,our Li‐O2 batteries offer excellent rate capability and ultra‐long cycling life of up to 210 cycles at 1000 mA/g under a fixed capacity of 1000 mA·h/g,which is two times longer than those of Pt@CNTs and PtNi@***,it is revealed that surface engineering of PtNi nanoalloy via B doping can efficiently tailor the electron structure of nanoalloy and optimize the adsorption of oxygen species,consequently delivering excellent Li‐O2 battery ***,this strategy of regulating the nanoalloy by doping nonmetallic elements will pave an avenue for the design of high‐performance catalysts for metal‐oxygen batteries.

关键词： B doping bifunctional catalyst Li‐O2 battery low charge overpotential PtNi nanoalloy

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2.4 V ultrahigh-voltage aqueous MXene-based asymmetric micro-supercapacitors with high volumetric energy density toward a self-sufficient integrated microsystem

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Fundamental Research 2024年第2期4卷 307-314页

作者： Yuanyuan Zhu Shuanghao Zheng Jieqiong Qin Jiaxin Ma Pratteek Das Feng Zhou Zhong-Shuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Shijingshan DistrictBeijing 100049China College of Science Henan Agricultural UniversityZhengzhou 450002China Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalian 116023China Key Laboratory of Spin Electron and Nanomaterials of Anhui Higher Education Institutes Suzhou UniversitySuzhou 234000China

Two-dimensional MXenes are key high-capacitance electrode materials for micro-supercapacitors(MSCs)catering to integrated ***,the narrow electrochemical voltage windows of conventional aqueous electrolytes(≤1.23 V)and symmetric MXene MSCs(typically≤0.6 V)substantially limit their output voltage and energy *** concentrated aqueous electrolytes exhibit lower water molecule activity,which inhibits water splitting and consequently widens the operating voltage ***,we report ultrahigh-voltage aqueous planar asymmetric MSCs(AMSCs)based on a highly concentrated LiCl-gel quasi-solid-state electrolyte with MXene(Ti3C2Tx)as the negative electrode and MnO_(2) nanosheets as the positive electrode(MXene//MnO_(2)-AMSCs).The MXene//MnO_(2)-AMSCs exhibit a high voltage of up to 2.4 V,attaining an ultrahigh volumetric energy density of 53 mWh cm−***,the in-plane geometry and the quasi-solid-state electrolyte enabled excellent mechanical flexibility and performance uniformity in the serially/parallel connected packs of our ***,the MXene//MnO_(2)-AMSC-based integrated microsystem,in conjunction with solar cells and consumer electronics,could efficiently realize simultaneous energy harvesting,storage,and *** findings of this study provide insights for constructing high-voltage aqueous MXene-based AMSCs as safe and self-sufficient micropower sources in smart integrated microsystems.

关键词： Asymmetric micro-supercapacitors MXene MnO_(2) Aqueous electrolyte High voltage Integrated microsystem

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SAPO-34 facilitates the formation of benzene,toluene and xylenes in direct syngas conversion over MnCrO_(x)-SAPO-34-ZSM-5

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Science China Chemistry 2024年第2期67卷 732-740页

作者： Shuchi Zhang Dengyun Miao Yi Ding Mengyuan Li Shujing Guo Yujuan Zhang Xiulian Pan Xinhe Bao State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China University of Chinese Academy of Sciences Beijing100049China Shaanxi Yanchang Petroleum(Group)Co. Ltd.&Dalian Institute of Chemical Physics Xi’an Clean Energy(Chemical Industry)Research InstituteXi’an710000China

Direct conversion of syngas to aromatics over metal oxide and zeolite(OXZEO) composite catalysts is ***,the selectivity of more valuable products such as benzene,toluene and xylenes(BTX) is limited due to undesired secondary methylation of ***,we report that the introduction of SAPO-34 into MnCrO_(x)-ZSM-5 catalyst enhances significantly the formation of BTX without sacrificing the aromatics *** optimized conditions,the fraction of BTX in aromatics reaches 64.7% versus 28.9% over the catalyst without SAPO-34.A number of model reaction tests and characterizations reveal that SAPO-34 consumes partially the intermediates such as ketene,by converting them to light ***,the methylation of BTX by ketene to heavy aromatics is inhibited over the external acid sites of ZSM-5,leading to an enhanced BTX selectivity in the *** hybrid catalyst provides an efficient method for highly selective synthesis of BTX from syngas.

关键词： selective syngas conversion OXZEO aromatics BTX multi-functional catalysts

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