Hao Xiaoqiong, An Xiaowei, Patil Amar M, Wang Peifen, Ma Xuli, Du Xiao, Hao Xiaogang, Abudula Abuliti, Guan Guoqing
Department of Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, China.
Energy Conversion Engineering Group, Institute of Regional Innovation (IRI), Hirosaki University, Matsubara, Aomori 030-0813, Japan.
ACS Appl Mater Interfaces. 2021 Jan 27;13(3):3738-3747. doi: 10.1021/acsami.0c13440. Epub 2021 Jan 17.
Conversion of CO into valuable chemicals via electrochemical CO reduction reaction (CORR) is a promising technology to alleviate the energy crisis and the greenhouse effect. Herein, low-cost wood biomass was applied as the carbon source to prepare nitrogen (N)-doped carbon electrocatalysts for the conversion of CO to CO and further as the cathode material for Zn-CO batteries. By virtue of N-doping and assistance of FeCl, a cedar biomass-derived three-dimensional (3D) N-doped graphitized carbon with a high N-doping content (5.38%), an ultrahigh specific surface area (1673.6 m g), rich nanopores, and sufficient active N sites was successfully obtained, which exhibited super CORR activity with a high faradaic efficiency of 91% at a low applied potential of 0.56 V (vs RHE) and a long-term stability for at least 20 h. Furthermore, a Zn-CO battery with it as the cathode material delivered a stable open circuit voltage of 0.79 V, a peak power density of 0.51 mW cm at 2.14 mA cm, and a maximum faradaic efficiency to CO of 80.4% at 2.56 mA cm, indicating that it could be applied in a practical process by using CO to generate power with the production of CO. Density functional theory calculations revealed that pyridinic N could more effectively decrease the free energy barriers for CORR and boost the reaction. This work not only revealed a facile approach to convert waste biomass into N-doped-graphitization carbon as valuable CORR electrocatalysts but also provided a new strategy to achieve "carbon solving carbon's problem".
通过电化学一氧化碳还原反应（CORR）将一氧化碳转化为有价值的化学品是缓解能源危机和温室效应的一项很有前景的技术。在此，低成本的木材生物质被用作碳源，制备用于将一氧化碳转化为一氧化碳的氮（N）掺杂碳电催化剂，并进一步用作锌-一氧化碳电池的阴极材料。借助于N掺杂和FeCl的辅助，成功获得了一种雪松生物质衍生的三维（3D）N掺杂石墨化碳，其具有高N掺杂含量（5.38%）、超高比表面积（1673.6 m²/g）、丰富的纳米孔和充足的活性N位点，在0.56 V（相对于可逆氢电极）的低施加电位下表现出超CORR活性，法拉第效率高达91%，并具有至少20小时的长期稳定性。此外，以其作为阴极材料的锌-一氧化碳电池在2.14 mA/cm²时提供了0.79 V的稳定开路电压、0.51 mW/cm²的峰值功率密度，在2.56 mA/cm²时对一氧化碳的最大法拉第效率为80.4%，表明它可以应用于利用一氧化碳发电并同时生产一氧化碳的实际过程中。密度泛函理论计算表明，吡啶型N可以更有效地降低CORR的自由能垒并促进反应。这项工作不仅揭示了一种将废弃生物质转化为有价值的CORR电催化剂的N掺杂石墨化碳的简便方法，还提供了一种实现“以碳解决碳问题”的新策略。
