Ye Jie, Hu Andong, Gao Chao, Li Fengqi, Li Lei, Guo Yulin, Ren Guoping, Li Bing, Rensing Christopher, Nealson Kenneth H, Zhou Shungui, Xiong Yujie
Fujian Provincial Key Laboratory of Soil Environmental Health and Regulation, College of Resources and Environment, Fujian Agriculture and Forestry University, Fuzhou, 350002, China.
School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, 230026, China.
Angew Chem Int Ed Engl. 2024 May 13;63(20):e202403884. doi: 10.1002/anie.202403884. Epub 2024 Apr 8.
Abiotic CH production driven by Fenton-type reactive oxygen species (ROS) has been confirmed to be an indispensable component of the atmospheric CH budget. While the chemical reactions independent of Fenton chemistry to ROS are ubiquitous in nature, it remains unknown whether the produced ROS can drive abiotic CH production. Here, we first demonstrated the abiotic CH production at the soil-water interface under illumination. Leveraging this finding, polymeric carbon nitrides (CN) as a typical analogue of natural geobattery material and dimethyl sulfoxide (DMSO) as a natural methyl donor were used to unravel the underlying mechanisms. We revealed that the ROS, photocatalytically produced by CN, can oxidize DMSO into CH with a high selectivity of 91.5 %. Such an abiotic CH production process was further expanded to various non-Fenton-type reaction systems, such as electrocatalysis, pyrocatalysis and sonocatalysis. This work provides insights into the geochemical cycle of abiotic CH, and offers a new route to CH production via integrated energy development.
由芬顿型活性氧（ROS）驱动的非生物甲烷生成已被证实是大气甲烷收支中不可或缺的组成部分。虽然自然界中与芬顿化学无关的化学反应普遍存在，但所产生的ROS是否能驱动非生物甲烷生成仍不清楚。在此，我们首次证明了光照下土壤-水界面的非生物甲烷生成。基于这一发现，使用作为天然地质电池材料典型类似物的聚合氮化碳（CN）和作为天然甲基供体的二甲基亚砜（DMSO）来揭示其潜在机制。我们发现，由CN光催化产生的ROS能够以91.5%的高选择性将DMSO氧化为甲烷。这种非生物甲烷生成过程进一步扩展到各种非芬顿型反应体系，如电催化、热催化和声催化。这项工作为非生物甲烷的地球化学循环提供了见解，并为通过综合能源开发生产甲烷提供了一条新途径。
