Synthesis of defect-rich La2O2CO3 supports for enhanced CO2-to-methanol conversion efficiency

Rui Zhang; Xiao Wang; Ke Wang; Huilin Wang; Xudong Sun; Weidong Shi; Shuyan Song; Hongjie Zhang

doi:10.1126/sciadv.adr3332

Synthesis of defect-rich La₂O₂CO₃ supports for enhanced CO₂-to-methanol conversion efficiency

Sci Adv. 2024 Dec 6;10(49):eadr3332. doi: 10.1126/sciadv.adr3332. Epub 2024 Dec 4.

Authors

Rui Zhang^{1

2}, Xiao Wang^{1

2}, Ke Wang^{1

2}, Huilin Wang^{1

2}, Xudong Sun^{1

2}, Weidong Shi³, Shuyan Song^{1

2}, Hongjie Zhang^{1

2

4}

Affiliations

¹ State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China.
² School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, China.
³ School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, China.
⁴ Department of Chemistry, Tsinghua University, Beijing 100084, China.

Abstract

Converting CO₂ 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 Cu⁰ 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_V) hinders CO₂ activation. Herein, we present a strategy by doping Nd into a La₂O₂CO₃ (LOC) support, enhancing O_V formation by disrupting its lattice dyadicity. This leads to higher Cu⁰ concentration and improved CO₂ 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 CO₂ conversion.