| 曹铭洋,刘冰,张泽会.Pd/Zn/C-N催化CO2加氢合成甲醇性能研究[J].分子催化,2023,37(5):473-483 |
| Pd/Zn/C-N催化CO2加氢合成甲醇性能研究 |
| The Study of CO2 Hydrogenation to Methanol over Pd/Zn/C-N Catalysts |
| 投稿时间：2023-05-16 修订日期：2023-07-03 |
| DOI：10.16084/j.issn1001-3555.2023.05.006 |
| 中文关键词: Pd Zn/C-N CO2 甲醇 |
| 英文关键词:Pd Zn/C-N CO2 methanol |
| 基金项目:国家自然科学基金 (22179148); 湖北省自然科学基金（2020CFA096） |
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| 中文摘要: |
| 利用Zn2+和2-甲基咪唑自组装形成的ZIF-8, 800 ℃ N2氮气气氛下焙烧得到Zn/C-N载体. 采用NaBH4还原法将不同含量Pd负载于Zn/C-N上焙烧后得到Pd/Zn/C-N催化剂, ICP测得 Pd实际负载量为0.02%、0.05%、0.1%、0.3%. 负载Pd后, 由于Pd氢溢流作用, ZnO表面还原温度降低, 氧空穴增加, 更有利于CO2解离吸附, 因此Pd负载量越高, 催化剂CO2转化率越高. 甲醇选择性受Pd纳米颗粒大小显著影响, 小颗粒Pd与ZnO相互作用更强, 更有利于甲醇生成, 其中0.02%Pd/Zn/C-N催化剂在275 ℃, 2 MPa反应条件下, Pd/g上甲醇时空收率最高, STYMeOH值为11.0 mol/(gPd·h). |
| 英文摘要: |
| ZIF-8 was formed by self-assembly of Zn2+ and 2-Methylimidazole. The Zn/C-N support are obtained by calcining at N2 atmosphere at 800 ℃ for 5 h. Pd was loaded onto Zn/C-N by using NaBH4 reduction method. The actual loading amount of Pd measured by ICP-OES were 0.02%, 0.05%, 0.1% and 0.3%. After loading Pd, the reduction temperature of surface ZnO decreased and oxygen vacancies increase due to Pd hydrogen spillover, which is more conducive to CO2 dissociation and adsorption. Therefore, the higher the Pd loading, the higher the CO2 conversion rate of the catalyst. The methanol selectivity is significantly affected by the size of Pd nanoparticles, and the interaction between small Pd particles and ZnO is stronger. This is more beneficial to generate methanol. The performance of the 0.02%Pd/Zn/C-N catalyst is the best at 275 ℃ and 2 MPa, and the methanol space-time yield is 11.0 mol/(gPd·h). |
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