Efficient utilization of nickel single atoms for CO2 electroreduction by constructing 3D interconnected nitrogen-doped carbon tube network
Efficient utilization of nickel single atoms for CO2 electroreduction by constructing 3D interconnected nitrogen-doped carbon tube network
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DOI：
10.1016/j.apcatb.2023.123083
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发表时间：
2023
期刊：
影响因子：
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通讯作者：
Kuiting Wang;Bin Chen;Y. Xuan;Wenjun Fan;Nan Sun;Shengho Chang;G. Meng
中科院分区：
文献类型：
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作者：
Kuiting Wang;Bin Chen;Y. Xuan;Wenjun Fan;Nan Sun;Shengho Chang;G. Meng
CO2电还原（CO2 RR）被广泛认为是实现碳中和的有效途径，而单原子催化剂（SACs）在CO2 RR中被证明是有效的。然而，大多数SAC由于其粉状特征而不能进一步放大性能。本文中，我们提出了许多孤立的镍单原子锚定在3D互连的N掺杂碳管（NiSAs@3D-INCT）网络作为自支撑电极。NiSAs@ 3D-INCT具有真正互连和高度有序的垂直和横向碳管通道，促进CO2相互作用和电解质传输。NiSAs@3D-INCT表现出优越的上级CO2 RR性能，在-0.96 V时的CO分电流密度为51.8 mA cm− 2，优于可逆氢电极（RHE）。X射线吸收精细结构谱和理论计算表明，NiSAs以Ni-N4构型负载在3D-INCT网络上，是CO2 RR的高活性位.这项工作将为CO2 RR开辟高性能SAC提供新的思路。
The CO2electroreduction (CO2RR) is extensively deemed as a promising route to reach carbon neutralization, while the single-atom catalysts (SACs) are proved to be effective in CO2RR. However, most SACs cannot further amplify performance due to their powdery feature. Herein, we present numerous isolated nickel single atoms anchored on 3D interconnected N-doped carbon tubes (NiSAs@3D-INCT) network as a self-supported electrode. The NiSAs@ 3D-INCT has truly interconnected and highly ordered vertical and lateral carbon tube-channels, which promote the CO2interaction and electrolyte transmission. The NiSAs@3D-INCT exhibits a superior CO2RR performance with an appreciable CO partial current density of 51.8 mA cm−2at − 0.96 Vversusthe reversible hydrogen electrode (RHE). X-ray absorption fine structure spectroscopy and theoretical computations reveal the NiSAs are loaded on the 3D-INCT network with Ni-N4configuration as highly active sites for CO2RR. This work will shed a new light on opening up high performance SACs for CO2RR.