Min Heewon, Kim Cheolho, Lin Shu-Ya, Choi Jiyun, Sim Yunjeong, Yu Bor-Yih, Moon Jun Hyuk
Department of Chemical and Biological Engineering, Korea University, 145 Anam-ro, Seongbuk-gu, Seoul, 02841, Republic of Korea.
Department of Chemical Engineering, National Taiwan University, Taipei, 106, Taiwan.
Adv Mater. 2025 Apr;37(16):e2418767. doi: 10.1002/adma.202418767. Epub 2025 Mar 25.
The electrochemical conversion of methane offers a sustainable alternative to traditional thermochemical syngas pathways; however, the rational design of catalysts that ensure high productivity remains a significant challenge. In this study, a high-entropy oxide (HEO) catalyst composed of Co, Cr, Fe, Mn, and Ni is explored, with a targeted element enriched, and identify that a Co-rich HEO demonstrates high efficiency in room-temperature electrochemical methane conversion. This analysis of the projected density of states (PDOS) reveals that Co sites in the HEO catalyst possess an optimally positioned p-band center for methane activation. The Co-rich HEO catalyst achieves an ethanol production rate of 12315 µmol/g/hr at 1.6 V, with a Faradaic efficiency of 63.5%; a flow cell electrolyzer equipped with this catalyst achieves continuous methane-to-ethanol conversion at a rate of 26533 µmol/g/hr over 100 h. Process modeling evaluates the economic and environmental implications, demonstrating that a commercially viable process can be realized through economies of scale while significantly reducing CO₂ emissions.
甲烷的电化学转化为传统热化学合成气途径提供了一种可持续的替代方案；然而，合理设计确保高生产率的催化剂仍然是一项重大挑战。在本研究中，探索了一种由钴、铬、铁、锰和镍组成的高熵氧化物（HEO）催化剂，并对其中一种元素进行了富集，结果表明富钴的HEO在室温电化学甲烷转化中表现出高效率。对态密度投影（PDOS）的分析表明，HEO催化剂中的钴位点具有用于甲烷活化的最佳p带中心位置。富钴的HEO催化剂在1.6 V电压下实现了12315 µmol/g/hr的乙醇产率，法拉第效率为63.5%；配备这种催化剂的流动池电解槽在100小时内实现了26533 µmol/g/hr的连续甲烷到乙醇转化。过程建模评估了经济和环境影响，表明通过规模经济可以实现商业上可行的过程，同时显著减少二氧化碳排放。
