Hu Chuangang, Paul Rajib, Dai Quanbin, Dai Liming
Australian Carbon Materials Centre (A-CMC), School of Chemical Engineering, University of New South Wales, Sydney, NSW 2052, Australia.
Department of Macromolecular Science and Engineering, Case School of Engineering, Case Western Reserve University, Cleveland, Ohio 44106, USA.
Chem Soc Rev. 2021 Nov 1;50(21):11785-11843. doi: 10.1039/d1cs00219h.
Since the discovery of N-doped carbon nanotubes as the first carbon-based metal-free electrocatalyst (C-MFEC) for oxygen reduction reaction (ORR) in 2009, C-MFECs have shown multifunctional electrocatalytic activities for many reactions beyond ORR, such as oxygen evolution reaction (OER), hydrogen evolution reaction (HER), carbon dioxide reduction reaction (CORR), nitrogen reduction reaction (NRR), and hydrogen peroxide production reaction (HOPR). Consequently, C-MFECs have attracted a great deal of interest for various applications, including metal-air batteries, water splitting devices, regenerative fuel cells, solar cells, fuel and chemical production, water purification, to mention a few. By altering the electronic configuration and/or modulating their spin angular momentum, both heteroatom(s) doping and structural defects (, atomic vacancy, edge) have been demonstrated to create catalytic active sites in the skeleton of graphitic carbon materials. Although certain C-MFECs have been made to be comparable to or even better than their counterparts based on noble metals, transition metals and/or their hybrids, further research and development are necessary in order to translate C-MFECs for practical applications. In this article, we present a timely and comprehensive, but critical, review on recent advancements in the field of C-MFECs within the past five years or so by discussing various types of electrocatalytic reactions catalyzed by C-MFECs. An emphasis is given to potential applications of C-MFECs for energy conversion and storage. The structure-property relationship for and mechanistic understanding of C-MFECs will also be discussed, along with the current challenges and future perspectives.
自2009年发现氮掺杂碳纳米管作为首个用于氧还原反应（ORR）的碳基金属无机电催化剂（C-MFEC）以来，C-MFEC对ORR以外的许多反应都表现出多功能电催化活性，如析氧反应（OER）、析氢反应（HER）、二氧化碳还原反应（CORR）、氮还原反应（NRR）和过氧化氢生产反应（HOPR）。因此，C-MFEC在各种应用中引起了极大的兴趣，包括金属空气电池、水分解装置、再生燃料电池、太阳能电池、燃料和化学品生产、水净化等等。通过改变电子构型和/或调节其自旋角动量，杂原子掺杂和结构缺陷（如原子空位、边缘）都已被证明能在石墨碳材料的骨架中产生催化活性位点。尽管某些C-MFEC已被制得与基于贵金属、过渡金属和/或其混合物的同类产品相当甚至更好，但为了将C-MFEC转化为实际应用，仍需要进一步的研究和开发。在本文中，我们通过讨论C-MFEC催化的各种类型的电催化反应，对过去五年左右C-MFEC领域的最新进展进行了及时、全面但批判性的综述。重点介绍了C-MFEC在能量转换和存储方面的潜在应用。还将讨论C-MFEC的结构-性能关系和机理理解，以及当前的挑战和未来的前景。
