标题: Unveiling a synergistic ZrO2-Ga2O3 promotion strategy for copper catalysts: Enhanced methanol synthesis from CO2 via improved hydrogenation of formate intermediate作者: Li, XZ (Li, Xiaozhong); Huang, J (Huang, Jia); Yuan, MW (Yuan, Mingwei); Zhao, YS (Zhao, Yushi); Li, MW (Li, Mengwei); Du, JW (Du, Jingwei); Li, JJ (Li, Jinjun); Wu, F (Wu, Feng); You, ZX (You, Zhixiong)
来源出版物: APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 卷: 382 文献号: 125970 DOI: 10.1016/j.apcatb.2025.125970 Early Access Date: SEP 2026 Published Date: 2026 MAR
摘要: Addressing the burgeoning energy and environmental imperatives by simultaneously enhancing the durability and methanol selectivity of Cu-based CO2 hydrogenation catalysts remains a formidable challenge. Here, we report the synthesis of 8Ga6Zr/Cu+ 80MA catalyst via a synergistic top-down (acid etching) and bottom-up (impregnation-deposition) synthetic strategy. The resultant catalyst manifests a spatial proximity "armor" comprising Ga- and Zr-oxide nanoparticles anchored onto the copper surface, thereby generating abundant oxide-Cu interfacial sites. It achieves a methanol space time yield of 349.3 gMeOH & sdot;kgcat 91.1 % under 1.0 MPa and 270 degrees C. The Ga2O3 and ZrO2 synergy enhances methanol selectivity by electronic modulation at oxide-Cu interfacial perimeter, optimizing CO2 adsorption geometry and inducing moderate electrophilicity at the carbon atom. This refines nucleophilic attack by activated hydrogen species, promoting bidentate formate (*bi-HCOO) formation and subsequent hydrogenation, thereby enhancing selective methanol production via a preferential formate pathway. This research provides a rational methodology for fabricating robust catalysts featuring active oxide-Cu sites, underscoring the importance of tailoring formate intermediate configuration in dictating CO2-to-methanol selectivity.
作者关键词: CO 2 hydrogenation; Oxide-Cu interface; Bidentate formate; Methanol synthesis
KeyWords Plus: CARBON-DIOXIDE; ACTIVE-SITES; HIGH-PERFORMANCE; CU; SURFACE; GAS; ADSORPTION; MODEL; ZNO; QUANTIFICATION
地址: [Li, Xiaozhong; Huang, Jia; Yuan, Mingwei; Zhao, Yushi; Li, Mengwei; Du, Jingwei; Li, Jinjun; Wu, Feng; You, Zhixiong] Wuhan Univ, Sch Resource & Environm Sci, Wuhan 430079, Peoples R China.
通讯作者地址: You, ZX (通讯作者)，Wuhan Univ, Sch Resource & Environm Sci, Wuhan 430079, Peoples R China.
电子邮件地址: [email protected]
影响因子：21.1
