Nickel single-atom catalysts intrinsically promoted by fast pyrolysis for selective electroreduction of CO2 into CO
Nickel single-atom catalysts intrinsically promoted by fast pyrolysis for selective electroreduction of CO2 into CO
复制标题
镍单原子催化剂本质上通过快速热解促进 CO2 选择性电还原为 CO
DOI：
10.1016/j.apcatb.2021.120997
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发表时间：
2022-05-01
期刊：
影响因子：
--
通讯作者：
Zhou, Zhen
中科院分区：
文献类型：
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作者：
Guo, Yibo;Yao, Sai;Zhou, Zhen
二氧化碳的电化学还原反应是实现碳中和的有效途径。由于最大化的原子利用率和优异的催化性能，单原子催化剂（SAC）预计对CO2 RR有效。在此，通过有效的快速热解制备氮掺杂的碳负载的Ni SAC（Ni-SAC@ NC）。Ni-SAC@ NC作为CO2 RR的电催化剂可以有效地将CO2转化为CO。在-0.6 ~-0.9 V（vs.可逆氢电极（RHE））的外加电位窗口内，法拉第效率保持在80%以上，在-0.6 V（vs. RHE）时最高FECO为95%。Ni-SAC@ NC可以在较小的过电位下实现最佳的CO选择性，超过大多数其他最先进的催化剂。计算结果还表明，Ni-N-3结构是活性中心。本工作不仅为SAC的制备提供了一条简单可行的新途径，而且证明了配位环境在电催化中的关键作用。
The electrochemical reduction reaction of carbon dioxide (CO2RR) is an effective way towards carbon neutralization. Single-atom catalysts (SACs) are expected to be efficient for CO2RR due to maximum atom utilization and excellent catalytic performance. Here, nitrogen-doped carbon supported Ni SACs (Ni-SAC@NCs) were prepared through effective fast pyrolysis. CO2 can convert into CO efficiently with Ni-SAC@NCs as electrocatalysts for CO2RR. The faradaic efficiency kept well above 80% in the applied potential window of -0.6 to -0.9 V (vs. reversible hydrogen electrode (RHE)), with a highest FECO of 95% at -0.6 V (vs. RHE). Ni-SAC@NCs can achieve the best CO selectivity under a small overpotential, surpassing most other state-of-the-art catalysts. Computations also indicate that the unique defect-Ni-N-3 structure is the active site. This work not only provides a simple and promising new route for the preparation of SACs, but also proves the key role of the coordination environment in electrocatalysis.