Zhao Wei, Mei Xueyi, Zhang Yexin, Zhang Zhenghui, Chen Kai, Xie Weiping, Xin Ying, Zhang Zhaoliang, Zhang Jian
Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, 1219 Zhongguan West Road, Ningbo 315201, People's Republic of China.
School of Chemistry and Chemical Engineering, University of Jinan, 336 West Road of Nan Xinzhuang, Jinan 250022, People's Republic of China.
Sci Adv. 2025 Jul 11;11(28):eadv1585. doi: 10.1126/sciadv.adv1585.
Dry reforming of methane (DRM) offers an attractive solution for the high-value utilization of two primary greenhouse gasses, methane and carbon dioxide, but its industrial applications are hindered by the net carbon dioxide-positive emissions resulting from substantial energy consumption. Here, we developed an electrified technology by passing electric current through a conductive catalyst constituting nickel and lanthanum(III) oxide cosupported on activated carbons, reaching thermodynamic equilibrium conversions and sustaining for at least 120 hours. Notably, the energy efficiency (2.976 millimoles per kilojoule) exceeds all the previously reported values, enabling net carbon dioxide-negative emissions powered by common sustainable electricity. An electrically driven release of lattice oxygen bridges the decomposition of the lanthanum oxycarbonate intermediate generated from carbon dioxide activation and the reduction of the resultant nickel oxide species by deposited carbon from methane dissociation, thus inhibiting excessive nickel oxidation and lanthanum(III) oxide carbonatation. The electrified approach would make DRM a true pathway mitigating overall carbon footprint and combating global warming.
甲烷干重整（DRM）为两种主要温室气体甲烷和二氧化碳的高价值利用提供了一个有吸引力的解决方案，但其工业应用受到大量能源消耗导致的净二氧化碳正排放的阻碍。在此，我们开发了一种电气化技术，通过使电流通过负载在活性炭上的镍和氧化镧（III）共负载的导电催化剂，达到热力学平衡转化率并持续至少120小时。值得注意的是，能量效率（每千焦2.976毫摩尔）超过了之前报道的所有值，实现了由普通可持续电力驱动的净二氧化碳负排放。晶格氧的电驱动释放弥合了由二氧化碳活化产生的碳酸镧中间体的分解与甲烷解离沉积的碳对所得氧化镍物种的还原之间的差距，从而抑制了过度的镍氧化和氧化镧（III）碳酸化。这种电气化方法将使DRM成为减轻整体碳足迹和应对全球变暖的真正途径。
