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A review of 3D monolithic carbon-based materials with a high photothermal conversion efficiency used for solar water vapor generation 用于太阳能水蒸气生成的高光热转换效率三维整体碳基材料综述
IF 5.7 3区 材料科学 Q2 Materials Science Pub Date : 2024-04-01 DOI: 10.1016/S1872-5805(24)60827-9
Yue Han , Peng Zhang , Xiaoming Zhao

In recent years, photothermal-driven desalination has been regarded as one of the most promising methods to solve the global crisis of freshwater scarcity. The solar generation of water vapor (SGWV) is a key process in seawater desalination which uses simple equipment and has a high cost-benefit. Among alternative photothermal conversion materials for a SGWV system, three-dimensional (3D) monolithic carbon-based materials have many advantages, including low cost, good structure control, and high light-harvesting efficiency which gives a high evaporation rate. 3D monolithic carbon-based materials with a high photothermal conversion efficiency are reviewed together with their use in interface SGWV. The working mechanism of SGWV and the classification of SGWV materials are first considered, followed by detailed consideration of 3D monolithic carbon materials, including their design, preparation and working mechanism in SGWV. Finally, both the advantages and disadvantages of 3D monolithic carbon materials with a high photothermal conversion efficiency are examined.

近年来,光热驱动海水淡化被认为是解决全球淡水匮乏危机最有前景的方法之一。太阳能产生水蒸气(SGWV)是海水淡化的关键过程,设备简单,成本效益高。在可用于 SGWV 系统的光热转换材料中,三维(3D)整体碳基材料具有许多优点,包括成本低、结构可控性好、光收集效率高,因而蒸发率高。本文综述了具有高光热转换效率的三维整体碳基材料及其在界面 SGWV 中的应用。首先介绍了 SGWV 的工作机制和 SGWV 材料的分类,然后详细介绍了三维整体碳材料,包括其设计、制备和在 SGWV 中的工作机制。最后,研究了具有高光热转换效率的三维整体碳材料的优缺点。
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引用次数: 0
Bismuth nanoparticles anchored on N-doped graphite felts to give stable and efficient iron-chromium redox flow batteries 锚定在掺杂 N 的石墨毡上的纳米铋粒子可产生稳定高效的铁铬氧化还原液流电池
IF 5.7 3区 材料科学 Q2 Materials Science Pub Date : 2024-02-01 DOI: 10.1016/S1872-5805(24)60837-1
Hang-xin Che , Yu-fei Gao , Jia-hui Yang , Song Hong , Lei-duan Hao , Liang Xu , Sana Taimoor , Alex W. Robertson , Zhen-yu Sun

Iron-chromium redox flow batteries (ICRFBs) use abundant and inexpensive chromium and iron as the active substances in the electrolyte and have great potential as a cost-effective and large-scale energy storage system. However, they are still plagued by several issues, such as the low electrochemical activity of Cr3+/Cr2+ and the occurrence of the undesired hydrogen evolution reaction (HER). We report the synthesis of amorphous bismuth (Bi) nanoparticles (NPs) immobilized on N-doped graphite felts (GFs) by a combined self-polymerization and wet-chemistry reduction strategy followed by annealing, which are used as the negative electrodes for ICRFBs. The resulting Bi NPs react with H+ to form intermediates and greatly inhibit the parasitic HER. In addition, the combined effect of Bi and N dopants on the surface of GF dramatically increases the electrochemical activity of Fe2+/Fe3+ and Cr3+/Cr2+, reduces the charge transfer resistance, and increases the mass transfer rate compared to plain GF. At the optimum Bi/N ratio of 2, a high coulombic efficiency of up to 97.7% is maintained even for 25 cycles at different current densities, the energy efficiency reaches 85.8% at 60.0 mA cm−2, exceeding many other reported materials, and the capacity reaches 862.7 mAh L−1 after 100 cycles, which is about 5.3 times that of bare GF.

铁铬氧化还原液流电池(ICRFBs)使用丰富而廉价的铬和铁作为电解液中的活性物质,作为一种经济高效的大规模储能系统具有巨大潜力。然而,它们仍然受到几个问题的困扰,如 Cr3+/Cr2+ 的电化学活性低和发生不希望发生的氢进化反应 (HER)。我们报告了采用自聚合和湿化学还原相结合的策略,在掺杂 N 的石墨毡 (GF) 上固定合成无定形铋 (Bi) 纳米粒子 (NPs),然后进行退火处理,并将其用作 ICRFB 的负极。生成的 Bi NPs 与 H+ 反应形成中间产物,极大地抑制了寄生 HER。此外,与普通 GF 相比,Bi 和 N 掺杂剂在 GF 表面的共同作用显著提高了 Fe2+/Fe3+ 和 Cr3+/Cr2+ 的电化学活性,降低了电荷转移电阻,并提高了传质速率。在最佳 Bi/N 比为 2 时,即使在不同的电流密度下循环 25 次,也能保持高达 97.7% 的高库仑效率;在 60.0 mA cm-2 时,能量效率达到 85.8%,超过了许多其他已报道的材料;循环 100 次后,容量达到 862.7 mAh L-1,约为裸 GF 的 5.3 倍。
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引用次数: 0
Defect engineering of carbon-based electrocatalysts for the CO2 reduction reaction: A review 用于二氧化碳还原反应的碳基电催化剂缺陷工程:综述
IF 5.7 3区 材料科学 Q2 Materials Science Pub Date : 2024-02-01 DOI: 10.1016/S1872-5805(24)60833-4
Yan-kun Lu, Bai-xue Cheng, Hao-yu Zhan, Peng Zhou

Electrocatalytic carbon dioxide (CO2) reduction is an important way to achieve carbon neutrality by converting CO2 into high-value-added chemicals using electric energy. Carbon-based materials are widely used in various electrochemical reactions, including electrocatalytic CO2 reduction, due to their low cost and high activity. In recent years, defect engineering has attracted wide attention by constructing asymmetric defect centers in the materials, which can optimize the physicochemical properties of the material and improve its electrocatalytic activity. This review summarizes the types, methods of formation and defect characterization techniques of defective carbon-based materials. The advantages of defect engineering and the advantages and disadvantages of various defect formation methods and characterization techniques are also evaluated. Finally, the challenges of using defective carbon-based materials in electrocatalytic CO2 reduction are investigated and opportunities for their use are discussed. It is believed that this review will provide suggestions and guidance for developing defective carbon-based materials for CO2 reduction.

电催化二氧化碳(CO2)还原是利用电能将二氧化碳转化为高附加值化学品,从而实现碳中和的重要途径。碳基材料因其低成本和高活性被广泛应用于各种电化学反应,包括电催化二氧化碳还原反应。近年来,通过在材料中构建不对称缺陷中心,从而优化材料的物理化学性质并提高其电催化活性的缺陷工程引起了广泛关注。本综述总结了缺陷碳基材料的类型、形成方法和缺陷表征技术。此外,还评估了缺陷工程的优势以及各种缺陷形成方法和表征技术的优缺点。最后,研究了在电催化二氧化碳还原中使用缺陷碳基材料所面临的挑战,并讨论了使用缺陷碳基材料的机遇。相信本综述将为开发用于二氧化碳还原的缺陷碳基材料提供建议和指导。
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引用次数: 0
A review of carbon-based catalysts and catalyst supports for simultaneous organic electro-oxidation and hydrogen evolution reactions 用于同时进行有机电氧化和氢气进化反应的碳基催化剂和催化剂载体综述
IF 5.7 3区 材料科学 Q2 Materials Science Pub Date : 2024-02-01 DOI: 10.1016/S1872-5805(24)60829-2
Zhi-dong Wang , Tian Xia , Zhen-hua Li , Ming-fei Shao

Producing organic electro-oxidation and hydrogen evolution reactions (HER) simultaneously in an electrolytic cell is an appealing method for generating valuable chemicals at the anode while also producing H2 at the cathode. Within this framework, the task of designing energy-saving electrocatalysts with high selectivity and stability is a considerable challenge. Carbon-based catalysts, along with their supports, have emerged as promising candidates due to their diverse sources, large specific surface area, high porosity and multidimensional characteristics. This review summarizes progress from 2012 to 2022, in the use of carbon-based catalysts and their supports for organic electrooxidation and HER. It delves into outer-sphere electrooxidation mechanisms involving molecule-mediated oxidation and oxidative radical coupling reactions, as well as inner-sphere electrooxidation mechanisms, encompassing both acidic and alkaline electrolytes. The review also explores prospective research directions within this domain, addressing various aspects such as the design of electrocatalytic materials, the study of the relationship between the structure and properties of electrocatalysts, as well as examining their potential industrial applications.

在电解池中同时进行有机电氧化反应和氢进化反应(HER)是一种很有吸引力的方法,既能在阳极产生有价值的化学物质,又能在阴极产生 H2。在此框架内,设计具有高选择性和稳定性的节能型电催化剂是一项相当大的挑战。碳基催化剂及其载体具有来源多样、比表面积大、孔隙率高和多维等特点,因此已成为前景广阔的候选催化剂。本综述总结了从 2012 年到 2022 年在使用碳基催化剂及其支持物进行有机电氧化和 HER 方面取得的进展。综述深入探讨了涉及分子介导氧化和氧化自由基偶联反应的外层电氧化机制,以及包括酸性和碱性电解质在内的内层电氧化机制。综述还探讨了这一领域的前瞻性研究方向,涉及电催化材料的设计、电催化剂结构与性能之间关系的研究以及其潜在的工业应用等各个方面。
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引用次数: 0
Cactus-like NC/CoxP electrode enables efficient and stable hydrogen evolution for saline water splitting 仙人掌状 NC/CoxP 电极可在盐水分离过程中实现高效稳定的氢进化
IF 5.7 3区 材料科学 Q2 Materials Science Pub Date : 2024-02-01 DOI: 10.1016/S1872-5805(24)60824-3
Xu Chen, Jin-yu Zhao, Wen-sheng Zhang, Xiao-min Wang

Designing efficient and robust catalysts for hydrogen evolution reaction (HER) is imperative for saline water electrolysis technology. A catalyst composed of CoxP nanowires array with N-doped carbon nanosheets (NC) was fabricated on Ni foam (NF) by an in-situ growth strategy. The material is designated as NC/CoxP@NF. In the preparation process, Co(OH)2 nanowires were transformed into a metal organic framework of cobalt (ZIF-67) on NF by the dissolution-coordination of endogenous Co2+ and 2-methylimidazole. The resulting cactus-like microstructure gives NC/CoxP@NF abundant exposed active sites and ion transport channels, which improve the HER catalytic reaction kinetics. Furthermore, the interconnected alternating nanowires and free-standing nanosheets in NC/CoxP@NF improve its structural stability, and the formation of surface polyanions (phosphate) and a NC nanosheet protective layer improve the anti-corrosive properties of catalysts. Thus, the NC/CoxP@NF has an excellent performance, requiring overpotentials of 107 and 133 mV for HER to achieve 10 mA cm−2 in 1.0 mol L−1 KOH and 1.0 mol L−1 KOH + 0.5 mol L−1 NaCl, respectively. This in-situ transformation strategy is a new way of constructing highly-efficient HER catalysts for saline water electrolysis.

设计高效、坚固的氢进化反应催化剂是盐水电解技术的当务之急。通过原位生长策略,在泡沫镍(NF)上制备了一种由 CoxP 纳米线阵列和掺杂 N 的碳纳米片(NC)组成的催化剂。该材料被命名为 NC/CoxP@NF。在制备过程中,Co(OH)2 纳米线通过内源 Co2+ 和 2-甲基咪唑的溶解配位转化为 NF 上的钴金属有机框架(ZIF-67)。由此形成的仙人掌状微结构赋予 NC/CoxP@NF 丰富的暴露活性位点和离子传输通道,从而改善了 HER 催化反应动力学。此外,NC/CoxP@NF 中相互连接的交替纳米线和独立的纳米片提高了其结构稳定性,表面多阳离子(磷酸盐)和 NC 纳米片保护层的形成提高了催化剂的抗腐蚀性能。因此,NC/CoxP@NF 具有优异的性能,在 1.0 mol L-1 KOH 和 1.0 mol L-1 KOH + 0.5 mol L-1 NaCl 条件下,HER 达到 10 mA cm-2 所需的过电位分别为 107 和 133 mV。这种原位转化策略是为盐水电解构建高效 HER 催化剂的一种新方法。
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引用次数: 0
MOF-derived nanocarbon materials for electrochemical catalysis and their advanced characterization 用于电化学催化的 MOF 衍生纳米碳材料及其高级表征
IF 5.7 3区 材料科学 Q2 Materials Science Pub Date : 2024-02-01 DOI: 10.1016/S1872-5805(24)60828-0
Xi Chen , Ming-xuan Li , Jin-lun Yan , Long-li Zhang

Because of the demand for clean and sustainable energy sources, nanocarbons, modified carbons and their composite materials derived from metal-organic frameworks (MOFs) are emerging as distinct catalysts for electrocatalytic energy conversion. These materials not only inherit the advantages of MOFs, like customizable dopants and structural diversity, but also effectively prevent the aggregation of nanoparticles of metals and metal oxides during pyrolysis. Consequently, they increase the electrocatalytic efficiency, improve electrical conductivity, and may play a pivotal role in green energy technologies such as fuel cells and metal-air batteries. This review first explores the carbonization mechanism of the MOF-derived carbon-based materials, and then considers 3 key aspects: intrinsic carbon defects, metal and non-metal atom doping, and the synthesis strategies for these materials. We also provide a comprehensive introduction to advanced characterization techniques to better understand the basic electrochemical catalysis processes, including mapping techniques for detecting localized active sites on electrocatalyst surfaces at the micro- to nano-scale and in-situ spectroscopy. Finally, we offer insights into future research concerning their use as electrocatalysts. Our primary objective is to provide a clearer perspective on the current status of MOF-derived carbon-based electrocatalysts and encourage the development of more efficient materials.

由于对清洁和可持续能源的需求,由金属有机框架(MOFs)衍生的纳米碳、改性碳及其复合材料正在成为电催化能源转换的独特催化剂。这些材料不仅继承了 MOFs 的优势,如可定制的掺杂剂和结构多样性,还能有效防止金属和金属氧化物纳米颗粒在热解过程中聚集。因此,它们能提高电催化效率,改善导电性,并可能在燃料电池和金属空气电池等绿色能源技术中发挥关键作用。本综述首先探讨了 MOF 衍生碳基材料的碳化机理,然后考虑了三个关键方面:内在碳缺陷、金属和非金属原子掺杂以及这些材料的合成策略。我们还全面介绍了先进的表征技术,以更好地了解基本的电化学催化过程,包括在微米到纳米尺度上检测电催化剂表面局部活性位点的制图技术和原位光谱学。最后,我们对未来将其用作电催化剂的研究提出了见解。我们的主要目标是为 MOF 衍生碳基电催化剂的现状提供一个更清晰的视角,并鼓励开发更高效的材料。
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引用次数: 0
Carbon-based electrocatalysts for water splitting at high-current-densities: A review 用于高电流密度水分离的碳基电催化剂:综述
IF 5.7 3区 材料科学 Q2 Materials Science Pub Date : 2024-02-01 DOI: 10.1016/S1872-5805(24)60831-0
Yu-xiang Chen , Xiu-hui Zhao , Peng Dong , Ying-jie Zhang , Yu-qin Zou , Shuang-yin Wang

Electrocatalytic water splitting is a promising strategy to generate hydrogen using renewable energy under mild conditions. Carbon-based materials have attracted attention in electrocatalytic water splitting because of their distinctive features such as high specific area, high electron mobility and abundant natural resources. Hydrogen produced by industrial electrocatalytic water splitting in a large quantity requires electrocatalysis at a low overpotential at a large current density. Substantial efforts focused on fundamental research have been made, while much less attention has been paid to the high-current-density test. There are many distinct differences in electrocatalysis to split water using low and high current densities such as the bubble phenomenon, local environment around active sites, and stability. Recent research progress on carbon-based electrocatalysts for water splitting at low and high current densities is summarized, significant challenges and prospects for carbon-based electrocatalysts are discussed, and promising strategies are proposed.

电催化水分裂是在温和条件下利用可再生能源制氢的一种前景广阔的策略。碳基材料具有高比表面积、高电子迁移率和丰富的自然资源等显著特点,因此在电催化水分离领域备受关注。通过工业电催化水分离大量生产氢气需要在大电流密度、低过电位条件下进行电催化。人们已经在基础研究方面做出了巨大努力,但对大电流密度试验的关注却少得多。使用低电流密度和高电流密度进行电催化分水有许多明显的不同,如气泡现象、活性位点周围的局部环境和稳定性。本文总结了在低电流密度和高电流密度条件下进行水分离的碳基电催化剂的最新研究进展,讨论了碳基电催化剂面临的重大挑战和前景,并提出了有前景的策略。
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引用次数: 0
Ir nanoclusters on ZIF-8-derived nitrogen-doped carbon frameworks to give a highly efficient hydrogen evolution reaction ZIF-8 衍生的掺氮碳框架上的 Ir 纳米团簇实现高效氢进化反应
IF 5.7 3区 材料科学 Q2 Materials Science Pub Date : 2024-02-01 DOI: 10.1016/S1872-5805(24)60832-2
Xi-ao Wang , Yan-shang Gong , Zhi-kun Liu , Pei-shan Wu , Li-xue Zhang , Jian-kun Sun

The precise change of the electronic structure of active metals using low-active supports is an effective way of developing high-performance electrocatalysts. The electronic interaction of the metal and support provides a flexible way of optimizing the catalytic performance. We have fabricated an efficient hydrogen evolution reaction (HER) electrocatalyst, in which Ir nanoclusters are uniformly loaded on a nitrogen-doped carbon framework (Ir@NC). The synthesis process entails immersing an annealed zeolitic imidazolate framework-8 (ZIF-8), prepared at 900 °C as a carbon source, into an IrCl3 solution, followed by a calcination-reduction treatment at 400 °C under a H2/Ar atmosphere. The three-dimensional porous structure of the nitrogen-doped carbon framework exposes more active metal sites, and the combined effect of the Ir clusters and the N-doped carbon support efficiently changes the electronic structure of Ir, optimizing the HER process. In acidic media, Ir@NC has a remarkable HER electrocatalytic activity, with an overpotential of only 23 mV at 10 mA cm−2, an ultra-low Tafel slope (25.8 mV dec−1) and good stability for over 24 h at 10 mA cm−2. The high activity of the electrocatalyst with a simple and scalable synthesis method makes it a highly promising candidate for the industrial production of hydrogen by splitting acidic water.

利用低活性支撑物精确改变活性金属的电子结构是开发高性能电催化剂的有效方法。金属与载体的电子相互作用为优化催化性能提供了灵活的途径。我们制备了一种高效的氢进化反应(HER)电催化剂,其中 Ir 纳米团簇均匀地负载在掺氮碳框架(Ir@NC)上。合成过程是将在 900 ℃ 下作为碳源制备的退火沸石咪唑酸盐框架-8(ZIF-8)浸入 IrCl3 溶液中,然后在 400 ℃ 的 H2/Ar 气氛下进行煅烧-还原处理。掺氮碳框架的三维多孔结构暴露了更多的活性金属位点,Ir 簇和掺氮碳支持物的共同作用有效地改变了 Ir 的电子结构,优化了 HER 过程。在酸性介质中,Ir@NC 具有显著的 HER 电催化活性,在 10 mA cm-2 的条件下过电位仅为 23 mV,具有超低的 Tafel 斜坡(25.8 mV dec-1),并且在 10 mA cm-2 的条件下可稳定运行 24 小时以上。该电催化剂的高活性以及简单、可扩展的合成方法,使其成为通过分离酸性水进行工业制氢的极具潜力的候选材料。
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引用次数: 0
Carbon-based metal-free nanomaterials for the electrosynthesis of small-molecule chemicals: A review 用于小分子化学品电合成的碳基无金属纳米材料:综述
IF 5.7 3区 材料科学 Q2 Materials Science Pub Date : 2024-02-01 DOI: 10.1016/S1872-5805(24)60836-X
Lei Shi , Yan-zhe Li , Hua-jie Yin , Shen-long Zhao

Electrocatalysis is a key component of many clean energy technologies that has the potential to store renewable electricity in chemical form. Currently, noble metal-based catalysts are most widely used for improving the conversion efficiency of reactants during the electrocatalytic process. However, drawbacks such as high cost and poor stability seriously hinder their large-scale use in this process and in sustainable energy devices. Carbon-based metal-free catalysts (CMFCs) have received growing attention due to their enormous potential for improving the catalytic performance. This review gives a concise comprehensive overview of recent developments in CMFCs for electrosynthesis. First, the fundamental catalytic mechanisms and design strategies of CMFCs are presented and discussed. Then, a brief overview of various electrosynthesis processes, including the synthesis of hydrogen peroxide, ammonia, chlorine, as well as various carbon- and nitrogen-based compounds is given. Finally, current challenges and prospects for CMFCs are highlighted.

电催化是许多清洁能源技术的关键组成部分,具有以化学形式储存可再生能源电力的潜力。目前,贵金属催化剂被广泛用于提高电催化过程中反应物的转化效率。然而,高成本和稳定性差等缺点严重阻碍了它们在这一过程和可持续能源设备中的大规模使用。碳基无金属催化剂(CMFCs)在提高催化性能方面具有巨大潜力,因此受到越来越多的关注。本综述简明扼要地全面概述了用于电合成的 CMFC 的最新发展。首先,介绍并讨论了 CMFCs 的基本催化机理和设计策略。然后,简要介绍了各种电合成工艺,包括过氧化氢、氨、氯以及各种碳基和氮基化合物的合成。最后,重点介绍了 CMFC 目前面临的挑战和前景。
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引用次数: 0
Graphene-based CO2 reduction electrocatalysts: A review 石墨烯基二氧化碳还原电催化剂:综述
IF 5.7 3区 材料科学 Q2 Materials Science Pub Date : 2024-02-01 DOI: 10.1016/S1872-5805(24)60839-5
Ze-lin Wu , Cong-wei Wang , Xiao-xiang Zhang , Quan-gui Guo , Jun-ying Wang

The reduction of carbon dioxide (CO2) by electrochemical methods for the production of fuels and value-added chemicals is an effective strategy for overcoming the global warming problem. Due to the stable molecular structure of CO2, the design of highly selective, energy-efficient and cost-effective electrocatalysts is key. For this reason, graphene and its derivatives are competitive for CO2 electroreduction with their unique and excellent physical, mechanical and electrical properties and relatively low cost. In addition, the surface of graphene-based materials can be modified using different methods, including doping, defect engineering, production of composite structures and wrapped shapes. We first review the fundamental concepts and criteria for evaluating electrochemical CO2 reduction, as well as the catalytic principles and processes. Methods for preparing graphene-based catalysts are briefly introduced, and recent research on them is summarized according to the categories of the catalytic sites. Finally, the future development direction of CO2 electroreduction technology is discussed.

利用电化学方法还原二氧化碳(CO2)以生产燃料和高附加值化学品,是解决全球变暖问题的有效策略。由于二氧化碳分子结构稳定,因此设计高选择性、高能效和高成本效益的电催化剂至关重要。因此,石墨烯及其衍生物以其独特而优异的物理、机械和电气性能以及相对较低的成本,在二氧化碳电还原方面具有很强的竞争力。此外,石墨烯基材料的表面可以通过不同的方法进行改性,包括掺杂、缺陷工程、生产复合结构和包裹形状。我们首先回顾了评估电化学二氧化碳还原的基本概念和标准,以及催化原理和过程。简要介绍了制备石墨烯基催化剂的方法,并根据催化位点的类别总结了近期的相关研究。最后,讨论了二氧化碳电还原技术的未来发展方向。
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引用次数: 0
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