Pan Binbin, Zhu Xiaorong, Wu Yunling, Liu Tongchao, Bi Xuanxuan, Feng Kun, Han Na, Zhong Jun, Lu Jun, Li Yafei, Li Yanguang
Institute of Functional Nano & Soft Materials (FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices Soochow University Suzhou 215123 China.
College of Chemistry and Materials Science Nanjing Normal University Nanjing 210023 China.
Adv Sci (Weinh). 2020 Jun 30;7(16):2001002. doi: 10.1002/advs.202001002. eCollection 2020 Aug.
There are growing interests in metal-free heteroatom-doped carbons for electrochemical CO reduction. Previous studies extensively focus on the effect of N-doping, and their products severely suffer from low current density (mostly <2 mA cm) and limited selectivity (<90%). Here, it is reported that heteroatom codoping offers a promising solution to the above challenge. As a proof of concept, N,P-codoped mesoporous carbon is prepared by annealing phytic-acid-functionalized ZIF-8 in NH. In CO-saturated 0.5 m NaHCO, the catalyst enables CO reduction to CO with great selectivity close to 100% and large CO partial current density (≈8 mA cm), which are, to the best of knowledge, superior to all other relevant competitors. Theoretical simulations show that the improved activity and selectivity are stemmed from the enhanced surface adsorption of *COOH and *CO intermediates as a result of the synergy of N and P codoping.
无金属杂原子掺杂碳在电化学CO还原方面的研究兴趣日益浓厚。以往的研究主要集中在氮掺杂的影响上，其产物严重存在电流密度低（大多<2 mA cm）和选择性有限（<90%）的问题。在此，据报道杂原子共掺杂为上述挑战提供了一个有前景的解决方案。作为概念验证，通过在NH中对植酸功能化的ZIF-8进行退火制备了N、P共掺杂的介孔碳。在CO饱和的0.5 m NaHCO中，该催化剂能够将CO还原为CO，选择性接近100%，且CO分电流密度大（≈8 mA cm），据所知，优于所有其他相关竞争者。理论模拟表明，活性和选择性的提高源于N和P共掺杂的协同作用导致COOH和CO中间体的表面吸附增强。
