Scholarlink

<p>We herein designed a double-atom catalyst based on 2D BC<sub>3</sub>N<sub>2</sub> and calculated the properties of CO<sub>2</sub>/CH<sub>4</sub> coactivation <i>via</i> density functional theory. PtM@2D-BC<sub>3</sub>N<sub>2</sub> catalysts (M denotes Cr, Mo, Ti, V, and W) are first screened based on high binding strength of metal atoms and CH<sub>4</sub> caputre ability. In these candidates, the systems with M in IVB and VB subgroups have unfavorable adsorption oritation of *CH<sub>3</sub>COO (*HCOO) for *CO<sub>2</sub>-*CH<sub>3</sub> (*CO<sub>2</sub>-*H) combination. In comparison, the systems with M in VIB subgroup are favourable and the reactivity of *CO<sub>2</sub>-*CH<sub>3</sub> (*CO<sub>2</sub>-*H) combination is decreased with increasing period. Finally, the PtCr@2D-BC<sub>3</sub>N<sub>2</sub> is screened as the optimal catalyst. There exists a synergistic effect between Pt and Cr sites in PtCr@2D-BC<sub>3</sub>N<sub>2</sub>: the CH<sub>4</sub> can be effectively adsorbed on Cr site and will further be dissociated on Pt site with high reactivity. HCOOH can be produced in the temperature region of 34.84–66.85 °C. While at temperatures higher than 66.85 °C, the selectivity of CH<sub>3</sub>COOH production is significantly higher than that of HCOOH due to the larger rate constant and ratio of atom utilization. Our study has not only clarified the potential mechanism of CO<sub>2</sub>/CH<sub>4</sub> coactivation for theoretical works but also provided promising candidates for experimental works.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Effective Coactivation of CO2 and CH4 Gases into HCOOH and CH3COOH Realized by Synergistic Effect in Double-atom Catalyst Based on 2D BC3N2

  • 期刊论文

  • 发表日期：

    2025年10月16日

查看全文
  • Xiao Wang,
  • Chaozheng He,
  • Chenxu Zhao

摘要

We herein designed a double-atom catalyst based on 2D BC3N2 and calculated the properties of CO2/CH4 coactivation via density functional theory. PtM@2D-BC3N2 catalysts (M denotes Cr, Mo, Ti, V, and W) are first screened based on high binding strength of metal atoms and CH4 caputre ability. In these candidates, the systems with M in IVB and VB subgroups have unfavorable adsorption oritation of *CH3COO (*HCOO) for *CO2-*CH3 (*CO2-*H) combination. In comparison, the systems with M in VIB subgroup are favourable and the reactivity of *CO2-*CH3 (*CO2-*H) combination is decreased with increasing period. Finally, the PtCr@2D-BC3N2 is screened as the optimal catalyst. There exists a synergistic effect between Pt and Cr sites in PtCr@2D-BC3N2: the CH4 can be effectively adsorbed on Cr site and will further be dissociated on Pt site with high reactivity. HCOOH can be produced in the temperature region of 34.84–66.85 °C. While at temperatures higher than 66.85 °C, the selectivity of CH3COOH production is significantly higher than that of HCOOH due to the larger rate constant and ratio of atom utilization. Our study has not only clarified the potential mechanism of CO2/CH4 coactivation for theoretical works but also provided promising candidates for experimental works.