Institute of Functional Material Chemistry, National & Local United Engineering Laboratory for Power Batteries, Northeast Normal University , Changchun, 130024 Jilin, People's Republic of China.
ACS Appl Mater Interfaces. 2017 Apr 5;9(13):11689-11695. doi: 10.1021/acsami.7b01721. Epub 2017 Mar 24.
Developing a photocatalysis system for converting CO to valuable fuels or chemicals is a promising strategy to address global warming and fossil fuel consumption. Exploring photocatalysts with high-performance and low-cost has been two ultimate goals toward photoreduction of CO. Herein, noble-metal-free polyoxometalates (Co4) with oxidative ability was first introduced into g-CN resulted in inexpensive hybrid materials (Co4@g-CN) with staggered band alignment. The staggered composited materials show a higher activity of CO reduction than bare g-CN. An optimized Co4@g-CN hybrid sample exhibited a high yield (107 μmol g h) under visible-light irradiation (λ ≥ 420 nm), meanwhile maintaining high selectivity for CO production (94%). After 10 h of irradiation, the production of CO reached 896 μmol g. Mechanistic studies revealed the introduction of Co4 not only facilitate the charge transfer of g-CN but greatly increased the surface catalytic oxidative ability. This work creatively combined g-CN with oxidative polyoxometalates which provide novel insights into the design of low-cost photocatalytic materials for CO reduction.
开发用于将 CO 转化为有价值燃料或化学品的光催化系统是解决全球变暖和化石燃料消耗的一种很有前途的策略。探索高性能和低成本的光催化剂一直是光还原 CO 的两个最终目标。本文首次将具有氧化能力的贵金属-free 多金属氧酸盐（Co4）引入 g-CN 中，得到了带隙排列的廉价杂化材料（Co4@g-CN）。与纯 g-CN 相比，交错复合材料表现出更高的 CO 还原活性。优化后的 Co4@g-CN 杂化样品在可见光照射下（λ≥420nm）表现出较高的 CO 生成产率（107 μmol g h），同时保持较高的 CO 选择性（94%）。在 10 小时的照射后，CO 的生成量达到了 896 μmol g。机理研究表明，Co4 的引入不仅促进了 g-CN 的电荷转移，而且极大地提高了表面催化氧化能力。这项工作创造性地将 g-CN 与氧化多金属氧酸盐结合在一起，为设计用于 CO 还原的低成本光催化材料提供了新的思路。
