Sunlight-driven photocatalysis is regarded as a promising strategy for direct conversion of methane in low concentration coal mine methane (LC-CMM) to value-added methanol, yet remains a grand challenge to efficiently activate and convert methane. Herein, WO_3−x nanosheets with gradient concentration of oxygen vacancy were synthesized and firstly served as full-spectrum responsive catalysts for transformation of LC-CMM to methanol at ambient conditions. Defect-rich WO_3−x-N2.0 shows a methanol yield of 1475 μmol·g⁻¹, roughly 4.5 times higher than WO₃-A2.0 under simulated solar light irradiation. The selectivity of CH₃OH on the optimal WO_3−x-N2.0 is up to 76%. More importantly, WO_3−x-N2.0 exhibits a methanol yield of 396 μmol·g⁻¹ with the selectivity of 82% even under near infrared light irradiation while almost no CH₃OH is detected over WO₃-A2.0. Based on the results of energy-band structure, photoelectrochemical characterization, PLs and EPR tests, the significantly enhanced photocatalytic performance over WO_3−x-N2.0 is ascribed to the synergistic effect caused by the formation of oxygen vacancies, including extending light absorption into NIR region, improving separation of photoinduced electron-hole pairs and boosting production of hydroxyl radicals (key active species that drive CH₃OH production). This work will offer a sustainable pathway to broaden the utilization of LC-CMM via efficient coupling of solar energy.

阳光驱动的光催化被认为是将低浓度煤矿瓦斯（LC-CMM）中的甲烷直接转化为高附加值甲醇的一种有前景的策略，但有效活化和转化甲烷仍然是一个巨大的挑战。在此，合成了具有梯度氧空位浓度的WO _3-x纳米片，并首先作为全光谱响应催化剂在环境条件下将 LC-CMM 转化为甲醇。在模拟太阳光照射下，富含缺陷的WO _3-x -N2.0 的甲醇产率为1475 μmol·g ^-1，大约是WO ₃ -A2.0 的4.5 倍。CH ₃ OH对最佳WO _3-x -N2.0的选择性高达76%。更重要的是，WO即使在近红外光照射下，_3-x -N2.0 也表现出396 μmol·g ^-1的甲醇产率和82% 的选择性，而在WO ₃ -A2.0 上几乎没有检测到CH ₃ OH 。基于能带结构、光电化学表征、PLs 和 EPR 测试的结果，WO _3-x -N2.0显着增强的光催化性能归因于氧空位形成引起的协同效应，包括延长光吸收进入 NIR 区域，改善光致电子-空穴对的分离并促进羟基自由基（驱动 CH _{3 的}关键活性物质）的产生OH 生产）。这项工作将提供一条可持续的途径，通过太阳能的有效耦合来扩大 LC-CMM 的利用。