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2024年  第39卷  第1期

2024年1期序言
2024, 39(1): 1-2.
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2024 年 1 期中文目次
2024, 39(1): 1-1.
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2024年1期英文目次
2024, 39(1): 1-5.
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综合评述
Carbon-based electrocatalysts for water splitting at high-current-densities: A review
CHEN Yu-xiang, ZHAO Xiu-hui, DONG Peng, ZHANG Ying-jie, ZOU Yu-qin, WANG Shuang-yin
2024, 39(1): 1-16. doi: 10.1016/S1872-5805(24)60831-0
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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.
Defect engineering of carbon-based electrocatalysts for the CO2 reduction reaction: A review
LU Yan-kun, CHENG Bai-xue, ZHAN Hao-yu, ZHOU Peng
2024, 39(1): 17-41. doi: 10.1016/S1872-5805(24)60833-4
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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.
Carbon-based metal-free nanomaterials for the electrosynthesis of small-molecule chemicals: A review
SHI Lei, LI Yan-zhe, YIN Hua-jie, ZHAO Shen-long
2024, 39(1): 42-63. doi: 10.1016/S1872-5805(24)60836-X
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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.
A review of carbon-based catalysts and catalyst supports for simultaneous organic electro-oxidation and hydrogen evolution reactions
WANG Zhi-dong, XIA Tian, LI Zhen-hua, SHAO Ming-fei
2024, 39(1): 64-77. doi: 10.1016/S1872-5805(24)60829-2
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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.
MOF-derived nanocarbon materials for electrochemical catalysis and their advanced characterization
CHEN Xi, LI Ming-xuan, Yan Jin-lun, Zhang Long-li
2024, 39(1): 78-99. doi: 10.1016/S1872-5805(24)60828-0
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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.
石墨烯基二氧化碳还原电催化材料研究进展
武泽林, 王聪伟, 张晓祥, 郭全贵, 王俊英
2024, 39(1): 100-130. doi: 10.1016/S1872-5805(24)60839-5
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通过电化学方法来减少二氧化碳(CO2),同时生产燃料和高附加值化学品,是一种克服全球变暖问题的有效策略,对于缓解能源和环境的双重压力具有重要的现实意义。由于CO2稳定的分子结构,设计高选择性、高能效和低成本的电催化剂是关键。石墨烯及其衍生物因其独特且优异的物理、力学和电学性能,相对较低的成本,使其在CO2电还原方面具有竞争力。此外,石墨烯基材料的表面可以通过使用不同的方法进行改性,包括掺杂、缺陷工程、构建复合结构和包覆形状。首先,本文综述了电化学CO2还原的基本概念、评价标准,以及催化原理和过程。其次,简要介绍了石墨烯基催化剂的制备方法,并按照催化位点的类别,总结了石墨烯基催化剂近年来的研究进展。最后,对CO2电还原技术未来发展方向进行了探讨与展望。

研究论文
Bismuth nanoparticles anchored on N-doped graphite felts to give stable and efficient iron-chromium redox flow batteries
CHE Hang-xin, GAO Yu-fei, YANG Jia-hui, HONG Song, HAO Lei-duan, XU Liang, Sana Taimoor, Alex W. Robertson, SUN Zhen-yu
2024, 39(1): 131-141. doi: 10.1016/S1872-5805(24)60837-1
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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.
A Co3O4/graphdiyne heterointerface for efficient ammonia production from nitrates
CHEN Zhao-yang, ZHAO Shu-ya, LUAN Xiao-yu, ZHENG Zhi-qiang, YAN Jia-yu, XUE Yu-rui
2024, 39(1): 142-151. doi: 10.1016/S1872-5805(24)60834-6
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The nitrate reduction reaction (NtRR) has been demonstrated to be a promising way for obtaining ammonia (NH3) by converting NO3 to NH3. Here we report the controlled synthesis of cobalt tetroxide/graphdiyne heterostructured nanowires (Co3O4/GDY NWs) by a simple two-step process including the synthesis of Co3O4 NWs and the following growth of GDY using hexaethynylbenzene as the precursor at 110 °C for 10 h. Detailed scanning electron microscopy, high resolution transmission electron microscopy, X-ray photoelectron spectroscopy, and Raman characterization confirmed the synthesis of a Co3O4/GDY heterointerface with the formation of sp-C―Co bonds at the interface and incomplete charge transfer between GDY and Co, which provide a continuous supply of electrons for the catalytic reaction and ensure a rapid NtRR. Because of these advantages, Co3O4/GDY NWs had an excellent NtRR performance with a high NH3 yield rate (YNH3) of 0.78 mmol h−1 cm−2 and a Faraday efficiency (FE) of 92.45% at −1.05 V (vs. RHE). This work provides a general approach for synthesizing heterostructures that can drive high-performance ammonia production from wastewater under ambient conditions.
Cactus-like NC/CoxP electrode enables efficient and stable hydrogen evolution for saline water splitting
CHEN Xu, ZHAO Jin-yu, ZHANG Wen-sheng, WANG Xiao-min
2024, 39(1): 152-163. doi: 10.1016/S1872-5805(24)60824-3
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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.
Ir nanoclusters on ZIF-8-derived nitrogen-doped carbon frameworks to give a highly efficient hydrogen evolution reaction
WANG Xi-ao, GONG Yan-shang, LIU Zhi-kun, WU Pei-shan, ZHANG Li-xue, SUN Jian-kun
2024, 39(1): 164-172. doi: 10.1016/S1872-5805(24)60832-2
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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.