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Catalytic conversion of C1 molecules under mild conditions 温和条件下C1分子的催化转化
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2021-01-01 DOI: 10.1016/j.enchem.2020.100050
Xiaoju Cui , Rui Huang , Dehui Deng

C1 catalysis based on the transformation of methane, carbon monoxide, methanol and carbon dioxide offers great potential for the sustainable production of fuels and chemicals in response to the decrease of the energy consumption and plant maintenance. While the relatively inert nature of CH and CO bond (e.g., methane and carbon dioxide) and uncontrollable coupling of CC bond render the selective activation and controllable transformation of C1 molecules to high-value-added products challenging in C1 chemistry. Catalytic conversion of C1 energy molecules under mild conditions enables a better control of the selectivity of the desired products, however, which requires highly active catalysts to lower the reaction energy barriers. Besides designing efficient catalysts to promote C1 molecules conversion, employing electro-catalysis and photo-catalysis to circumvent the thermodynamic limitations is regarded as promising ways for C1 catalysis at low temperatures. Benefiting from the advanced technology for catalyst synthesis, reactor design, mechanism understanding, catalytic conversion of C1 molecules under mild conditions has made significant progress from 2010 to 2020. In this review, we summarized the typical catalytic processes and representative catalysts for transforming methane, carbon monoxide, methanol and carbon dioxide into high value-added chemicals with a reaction temperatures below 200 °C driven by thermo-catalysis, electro-catalysis, and photo-catalysis. Besides, a short perspective is offered to highlight possible future research directions towards C1 molecules conversion under mild conditions. It is expected to provide a useful reference for the readers to design better catalysts and reaction process for mild conversion of C1 molecules efficiently in future.

基于甲烷、一氧化碳、甲醇和二氧化碳转化的C1催化为燃料和化学品的可持续生产提供了巨大的潜力,以响应能源消耗和工厂维护的减少。而CH和CO键(如甲烷和二氧化碳)的相对惰性和CC键的不可控偶联使得C1分子的选择性活化和可控转化为高附加值产品在C1化学中具有挑战性。C1能量分子在温和条件下的催化转化可以更好地控制所需产物的选择性,但这需要高活性催化剂来降低反应能垒。除了设计高效催化剂促进C1分子转化外,利用电催化和光催化绕过热力学限制被认为是C1低温催化的有前途的途径。得益于催化剂合成、反应器设计、机理理解等方面的先进技术,2010年至2020年,C1分子在温和条件下的催化转化取得了重大进展。本文综述了热催化、电催化和光催化在200℃以下反应条件下将甲烷、一氧化碳、甲醇和二氧化碳转化为高附加值化学品的典型催化过程和具有代表性的催化剂。并对未来可能的温和条件下C1分子转化研究方向进行了展望。希望能为今后设计更好的催化剂和反应工艺,实现C1分子的高效温和转化提供有益的参考。
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引用次数: 32
Covalent organic framework based lithium-ion battery: Fundamental, design and characterization 基于共价有机框架的锂离子电池:基础、设计和表征
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2021-01-01 DOI: 10.1016/j.enchem.2020.100048
Yiming Hu , Lacey J. Wayment , Catherine Haslam , Xiye Yang , Se-hee Lee , Yinghua Jin , Wei Zhang

Lithium-ion batteries have become a staple in modern technology. Development of the next-generation batteries with higher energy storage capacity, light weight, and long lifetime is highly dependent on the advancement of novel materials utilized in each battery component. A recently emerging approach has been to utilize Covalent Organic Frameworks (COFs) to rationally design cathode, anode, and electrolyte materials for LIBs. COFs have many desirable properties, such as porosity, robust backbone, and customizable structure, for applications in LIBs. In this review, we discuss the electrochemical characterization of lithium ion batteries, general COF design principles, and examples of COF-based cathodes, anodes, and electrolytes to highlight the great potential and current obstacles in this rapidly developing field.

锂离子电池已经成为现代科技的重要组成部分。下一代电池的发展具有更高的能量存储容量,重量轻,寿命长,高度依赖于每个电池组件所使用的新材料的进步。最近出现的一种方法是利用共价有机框架(COFs)来合理设计锂离子电池的阴极、阳极和电解质材料。COFs具有许多理想的特性,如多孔性、坚固的骨架和可定制的结构,适用于lib中的应用。在这篇综述中,我们讨论了锂离子电池的电化学特性,COF的一般设计原则,以及基于COF的阴极、阳极和电解质的例子,以突出这一快速发展领域的巨大潜力和当前的障碍。
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引用次数: 56
Bimetallic nanoparticles as cocatalysts for versatile photoredox catalysis 双金属纳米颗粒作为多用途光氧化还原催化的助催化剂
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2021-01-01 DOI: 10.1016/j.enchem.2020.100047
Yue-Hua Li , Jing-Yu Li , Yi-Jun Xu

Semiconductor photocatalysis is considered as a cutting-edge research topic for the production of value-added fuels and chemicals to confront the global energy crisis. In order to improve the solar-to-chemical conversion efficiency of pristine semiconductors, combining them with cocatalysts to form heterostructures has been extensively investigated. Among studied formulations, bimetallic nanoparticles (NPs), featuring enhanced light harvesting, efficient capture of photogenerated electrons and abundant surface active sites are ideal cocatalysts to improve the photocatalytic performance of semiconductor-based photocatalysts. In this review, we begin with a concise overview of representative synthesis and characterization methods of bimetallic NPs. Then, we predominantly summarize the typical applications of semiconductor/bimetallic NPs-based composites in photoredox catalysis, including hydrogen evolution, carbon dioxide reduction, selective organic synthesis and environmental remediation. In particular, we highlight the regulatory effects of parameters of bimetallic NPs (composition, structure, morphology, size, atomic arrangement, loading position, etc.) on the photocatalytic activity and selectivity. Finally, the remaining challenges and future perspectives for the utilization of bimetallic NPs in photoredox catalysis are discussed and anticipated to stimulate the sparkling ideas in the construction of high-efficiency semiconductor/bimetallic NPs-based photocatalytic systems.

半导体光催化被认为是生产高附加值燃料和化学品以应对全球能源危机的前沿研究课题。为了提高原始半导体的光化学转换效率,将其与助催化剂结合形成异质结构已被广泛研究。在所研究的配方中,双金属纳米颗粒(NPs)具有强光捕获、高效捕获光生电子和丰富的表面活性位点的特点,是提高半导体基光催化剂光催化性能的理想助催化剂。在这篇综述中,我们首先简要概述了代表性的双金属NPs的合成和表征方法。然后,重点总结了半导体/双金属nps基复合材料在光氧化还原催化中的典型应用,包括析氢、二氧化碳还原、选择性有机合成和环境修复。特别地,我们强调了双金属NPs的参数(组成、结构、形态、尺寸、原子排列、负载位置等)对光催化活性和选择性的调节作用。最后,讨论了双金属NPs在光氧化还原催化中的应用所面临的挑战和未来的前景,并展望了基于半导体/双金属NPs的高效光催化体系的构建。
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引用次数: 91
Recent advances in stability of organic solar cells 有机太阳能电池稳定性研究进展
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2021-01-01 DOI: 10.1016/j.enchem.2020.100046
Xiang Xu , Dongxu Li , Jun Yuan , Yonghua Zhou , Yingping Zou

Organic solar cells have achieved rapid development over the last few years, benefitting from the emerging of new non-fullerene acceptors (NFAs). The reported power conversion efficiency of OSCs has achieved over 18% up to now, however, the inferior stability issue restricts its commercialization, which stimulates the interest of scientists to explore it in-depth as well. Thus, we discuss the mechanisms of the instability in OSC devices, comprehensively summarize the progress of OSC stability in recent years and propose a series of solutions that improve the stability in this review. Although the highly-stable OSCs with extrapolated lifetime over several decades have been reported, the biggest drawback of them is the insufficient PCE. Thereby, investigating efficient OSCs with high-stability is required. We expect this review can provide some guidelines to address the instability of OSCs for feasible commercialization in the future.

近年来,新型非富勒烯受体(non-fullerene receptor, nfa)的出现使有机太阳能电池取得了飞速的发展。目前已报道的OSCs功率转换效率已达到18%以上,但稳定性差的问题限制了其商业化,这也激发了科学家对其深入探索的兴趣。因此,本文讨论了盐酸盐器件的不稳定性机制,全面总结了近年来盐酸盐稳定性的研究进展,并提出了一系列提高盐酸盐器件稳定性的解决方案。虽然已经报道了高稳定的OSCs,其外推寿命超过几十年,但其最大的缺点是PCE不足,因此需要研究具有高稳定性的高效OSCs。我们希望这篇综述可以为解决osc的不稳定性提供一些指导,以便将来可行的商业化。
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引用次数: 36
Recent advances on TiO2-based photocatalytic CO2 reduction 二氧化钛光催化CO2还原研究进展
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2020-11-01 DOI: 10.1016/j.enchem.2020.100044
Stefanie Kreft, Wei Duo, Henrik Junge, Matthias Beller

The sufficient supply of energy remains one of the most important challenges for a sustainable development of our society. In this respect, capturing sunlight energy by photocatalytic reduction of the greenhouse gas CO2 is interesting. In a more general way, the smart use of CO2 as C1-feedstock and its conversion to valuable carbon-based materials and energy sources can be the basis to establish a closed-CO2 cycle. This review summarizes recent advances in photocatalytic utilization of CO2 catalyzed by most prominent TiO2 based systems. The influences of different structures (i.e. crystal phase, morphology, vacancies, and defects), co-catalysts, and reaction conditions onto the catalyst performance are specifically highlighted. Furthermore, the reader attention is drawn to the oxidation counter reaction, which has been often neglected in the past.

充足的能源供应仍然是我们社会可持续发展的最重要挑战之一。在这方面,通过光催化减少温室气体二氧化碳来捕获太阳能是很有趣的。更一般地说,巧妙地利用二氧化碳作为c1原料,并将其转化为有价值的碳基材料和能源,可以成为建立一个封闭的二氧化碳循环的基础。本文综述了近年来主要的TiO2基体系在CO2光催化利用方面的研究进展。特别强调了不同结构(即晶相、形貌、空位和缺陷)、助催化剂和反应条件对催化剂性能的影响。此外,读者的注意力被吸引到氧化对抗反应,这在过去经常被忽视。
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引用次数: 39
Recent progress and perspectives of defective oxide anode materials for advanced lithium ion battery 先进锂离子电池缺陷氧化物负极材料研究进展与展望
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2020-11-01 DOI: 10.1016/j.enchem.2020.100045
Chenlong Dong , Wujie Dong , Xueyu Lin , Yantao Zhao , Ruizhe Li , Fuqiang Huang

Lithium ion batteries (LIBs) have become an indispensable part of human development and our lives, from spaceships to deep-sea submersibles as well as ordinary electronics. Since it was proposed in the 1970s and commercialized in 1991, LIBs have been pursuing higher energy, higher power, higher safety and higher durability. Therefore, there is an urgent need to develop more efficient anode materials to overcome the capacity and rate bottlenecks of commercial graphite. Oxide anodes stand out in terms of high capacity and working potential, e.g., Li4Ti5O12 has been a high-performance safe anode material. Yet developed early, most of oxide anodes suffer from low conductivity, low initial coulombic efficiency and large volume change during lithium/delithiation process. Recently, defect engineering has significantly improved the performance of oxide anodes and alleviated the above problems. In this review, we present the fundamentals, challenges and recent research progress on defective oxide anodes of LIBs. Firstly, the development history of LIBs and oxide anode is briefly introduced. Then, the definition, classification, preparation method, structure-function relationship between defect structure and electrochemical performance are introduced in detail, as well as the development perspective of defect oxide anode.

从宇宙飞船到深海潜水器,再到普通的电子产品,锂离子电池已经成为人类发展和生活中不可或缺的一部分。自20世纪70年代提出并于1991年商业化以来,lib一直在追求更高的能量、更高的功率、更高的安全性和更高的耐用性。因此,迫切需要开发更高效的阳极材料来克服商用石墨的容量和速率瓶颈。氧化阳极在高容量和工作潜力方面表现突出,例如Li4Ti5O12是一种高性能的安全阳极材料。大多数氧化阳极发展较早,存在电导率低、初始库仑效率低、锂/锂耗过程体积变化大等问题。近年来,缺陷工程使氧化阳极的性能得到了显著提高,上述问题得到了缓解。本文综述了锂离子电池缺陷阳极的基本原理、面临的挑战以及近年来的研究进展。首先,简要介绍了锂离子电池和氧化阳极的发展历史。然后详细介绍了缺陷氧化物阳极的定义、分类、制备方法、缺陷结构与电化学性能之间的结构-功能关系以及缺陷氧化物阳极的发展前景。
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引用次数: 35
Unique structural advances of graphdiyne for energy applications 石墨炔在能源应用方面的独特结构进步
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2020-09-01 DOI: 10.1016/j.enchem.2020.100041
Yasong Zhao , Nailiang Yang , Ranbo Yu , Yue Zhang , Jin Zhang , Yuliang Li , Dan Wang

Different from other carbon allotropes, graphdiyne (GDY) features topological sp- and sp2-hybridized carbon atoms. With the unique structural advances, a charming electronic behavior has been presented by GDY, which has shown great improvement for various energy-related fields. Inspired by this, it is time to summarize the structure-induced property enhancement. Firstly, different stacking configurations in GDY can induce specific electronic properties, bringing promising energy application. Secondly, uniform pores provide enough sites for anchoring atoms and nanoparticles, enriching the diversity of materials. Thirdly, the sufficient alkynyl groups offer active sites for doping and grafting, providing possibilities for the precise design at the molecular level. Lastly, we propose some perspectives for future trends on GDY. Through this review, we hope to provide a guideline for rational design on GDY-based materials and reveal the structure-performance relationship between functionalized GDY and energy conversion/storage.

与其他碳同素异形体不同,石墨炔(GDY)具有sp-和sp2杂化碳原子的拓扑特征。GDY以其独特的结构进步,呈现出迷人的电子行为,在能源相关的各个领域显示出巨大的进步。受此启发,是时候总结一下结构诱导的性能增强了。首先,GDY中不同的堆叠构型可以诱导出特定的电子性质,具有很好的能量应用前景。其次,均匀的孔隙为原子和纳米粒子提供了足够的锚定位点,丰富了材料的多样性。第三,充分的炔基为掺杂和接枝提供了活性位点,为分子水平上的精确设计提供了可能。最后,对GDY的未来发展趋势提出了展望。通过这一综述,我们希望为GDY基材料的合理设计提供指导,并揭示功能化GDY与能量转换/存储之间的结构-性能关系。
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引用次数: 37
Hole (donor) and electron (acceptor) transporting organic semiconductors for bulk-heterojunction solar cells 块状异质结太阳能电池中传输有机半导体的空穴(供体)和电子(受体)
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2020-09-01 DOI: 10.1016/j.enchem.2020.100042
Jianhua Chen , Yao Chen , Liang-Wen Feng , Chunling Gu , Guoping Li , Ning Su , Gang Wang , Steven M. Swick , Wei Huang , Xugang Guo , Antonio Facchetti , Tobin J. Marks

The field of bulk heterojunction (BHJ) organic photovoltaics (OPVs) or solar cells (OSCs) has experienced a dramatic advance toward a competitive technology reflecting the introduction of new materials, tuning of materials combinations, and optimization of the device architecture. Thus, binary BHJ OSCs with power conversion efficiencies surpassing 18% have been demonstrated. In this review we discuss recent developments in the area of π-conjugated small-molecule and polymeric semiconductors for organic BHJ-OSCs focusing on both electron-donor (hole-transporting) and electron-acceptor (electron-transporting) semiconductors developed during the past three years. Thus, several families of semiconductor materials including donor-acceptor (D-A) polymers, fullerene, and non-fullerene acceptors (NFAs) are reviewed including their combination for polymer-fullerene, donor polymer-NFA, all-small molecule, and all-polymer solar cells.

体异质结(BHJ)有机光伏(opv)或太阳能电池(OSCs)领域已经经历了一个戏剧性的进步,向竞争技术反映了新材料的引入,材料组合的调整,以及器件架构的优化。因此,已经证明了功率转换效率超过18%的二元BHJ osc。本文综述了近年来π共轭小分子半导体和聚合物半导体在有机BHJ-OSCs中的研究进展,重点介绍了近三年来电子给体(空穴传递)和电子受体(电子传递)半导体的研究进展。因此,综述了几种半导体材料家族,包括给体-受体(D-A)聚合物、富勒烯和非富勒烯受体(nfa),包括它们在聚合物-富勒烯、给体聚合物- nfa、全小分子和全聚合物太阳能电池中的组合。
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引用次数: 40
Nitrogen-doped nanostructured carbons: A new material horizon for water desalination by capacitive deionization 氮掺杂纳米碳:电容去离子海水淡化的新材料领域
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2020-09-01 DOI: 10.1016/j.enchem.2020.100043
Xingtao Xu , Shuaihua Zhang , Jing Tang , Likun Pan , Miharu Eguchi , Jongbeom Na , Yusuke Yamauchi

Capacitive deionization (CDI) is regarded as a novel, low-cost, and environmentally friendly technique that plays a critical role in desalination and water treatment. Although much progress has been achieved, the development of better CDI technologies, especially through the design and synthesis of various porous carbonaceous materials with enhanced CDI performance, continues to attract increasing interest within the scientific fraternity. Considering that previous traditional porous carbons might suffer from deficient salt adsorption capacity, the nitrogenization of porous carbons, which brings new opportunities for CDI applications, has emerged as an effective strategy to modify the surface characteristics of porous carbons and ultimately improve their CDI performance. This review summarizes the recent significant breakthroughs on the construction of NCs, including in situ doping and post-treatment strategies, and their practices in the field of CDI to impart a comprehensive understanding of the strategic evolution of the synthetic approaches to nitrogen-doped carbons (NCs) with remarkable CDI characteristics. We present an exhaustive analysis of newly synthesized NCs and the impact of their compositional and structural features on their CDI performance; further, we highlight a special emphasis on the possible role of nitrogen dopants in the CDI process. In addition to elucidating the state-of-the-art CDI applications, we address the remaining challenges, and finally, the possible direction for the use of NCs for CDI is described to provide some useful clues for future developments in this promising field.

电容去离子(CDI)是一种新型、低成本、环保的技术,在海水淡化和水处理中发挥着重要作用。尽管已经取得了很大的进展,但更好的CDI技术的发展,特别是通过设计和合成具有增强CDI性能的各种多孔碳质材料,继续吸引科学界越来越多的兴趣。考虑到以往传统多孔碳的吸盐能力不足,对多孔碳进行氮化处理是改变多孔碳表面特性,最终提高其CDI性能的一种有效策略,为CDI的应用带来了新的机遇。本文综述了近年来国内外在原位掺杂、后处理等碳纳米管构建方面的重大突破,以及在碳纳米管领域的实践,以全面了解具有显著碳纳米管特性的氮掺杂碳纳米管合成方法的策略演变。我们详细分析了新合成的nc及其组成和结构特征对其CDI性能的影响;此外,我们特别强调氮掺杂剂在CDI过程中的可能作用。除了阐明最先进的CDI应用之外,我们还解决了剩余的挑战,最后,描述了在CDI中使用nc的可能方向,为这个有前途的领域的未来发展提供了一些有用的线索。
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引用次数: 69
Multifunctional porous aromatic frameworks: State of the art and opportunities 多功能多孔芳香框架:现状和机遇
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2020-09-01 DOI: 10.1016/j.enchem.2020.100037
Ye Yuan, Yajie Yang, Guangshan Zhu

Porous aromatic frameworks (PAFs) are amorphous porous materials that are known for their large surface area, versatile structure, and high thermal/chemical stability. PAFs are constructed via a bottom-up approach from rigid organic building units that have a predesigned geometry and are connected through irreversible CC bonds. Due to their intriguing and tailorable structures, PAFs are widely deployed in catalysis, ion/molecule storage, and many other valuable applications. This review summarizes the recent progress on PAFs and PAF derivatives, including their design, synthesis, and applications. We conduct a detailed correlation investigation between the structural and chemical features of PAFs and their potential functions. The significant advantages (and disadvantages) and opportunities of PAFs are also discussed for the development of next-generation porous materials in the future for practical applications.

多孔芳香骨架(paf)是一种非晶多孔材料,以其大表面积、多用途结构和高热/化学稳定性而闻名。paf是由刚性有机建筑单元自下而上构建的,这些单元具有预先设计的几何形状,并通过不可逆的C - C键连接。由于其有趣和可定制的结构,paf被广泛应用于催化、离子/分子存储和许多其他有价值的应用。本文综述了PAF及其衍生物的设计、合成和应用等方面的研究进展。我们对paf的结构和化学特征及其潜在功能进行了详细的相关性研究。讨论了paf的显著优点(缺点)和机会,为未来开发下一代多孔材料的实际应用提供了参考。
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引用次数: 26
期刊
EnergyChem
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