Zhang Rui, Wang Xiao, Wang Ke, Wang Huilin, Sun Xudong, Shi Weidong, Song Shuyan, Zhang Hongjie
State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China.
School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, China.
Sci Adv. 2024 Dec 6;10(49):eadr3332. doi: 10.1126/sciadv.adr3332. Epub 2024 Dec 4.
Converting CO to methanol is crucial for addressing fuel scarcity and mitigating the greenhouse effect. Cu-based catalysts, with their diverse surface states, offer the potential to control reaction pathways and generate reactive H* species. However, a major challenge lies in oxidizing active Cu species by water generated during the catalytic process. While nonreducible metal oxides are beneficial in stabilizing metallic states, their limited capability to generate surface oxygen vacancies (O) hinders CO activation. Herein, we present a strategy by doping Nd into a LaOCO (LOC) support, enhancing O formation by disrupting its lattice dyadicity. This leads to higher Cu concentration and improved CO activation. The resulting Cu/LOC:Nd catalyst notably outperforms Cu/LOC and CuZnAl catalysts, achieving a methanol yield of 9.9 moles of methanol per hour per mole of Cu. Our approach opens up possibilities for enhancing Cu-based catalysts in CO conversion.
将一氧化碳转化为甲醇对于解决燃料短缺和减轻温室效应至关重要。具有多种表面状态的铜基催化剂具有控制反应路径和产生活性氢*物种的潜力。然而,一个主要挑战在于催化过程中产生的水会氧化活性铜物种。虽然不可还原的金属氧化物有利于稳定金属状态,但其产生表面氧空位(O)的能力有限,阻碍了一氧化碳的活化。在此,我们提出一种通过将钕掺杂到LaOCO(LOC)载体中的策略,通过破坏其晶格二元性来增强氧的形成。这导致更高的铜浓度和改善的一氧化碳活化。所得的Cu/LOC:Nd催化剂明显优于Cu/LOC和CuZnAl催化剂,每摩尔铜每小时的甲醇产率达到9.9摩尔。我们的方法为增强铜基催化剂在一氧化碳转化中的性能开辟了可能性。