MOF衍生的铜氮掺杂碳复合材料：N型和铜对选择性CO <sub>2</sub>电还原的协同作用<a href="#fn1" title="可用的电子补充信息（ESI）：详细的测试方法；图S1-S20和表S1-S3。参见DOI：10.1039 / c9cy01131e">†</a>,Catalysis Science & Technology

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MOF衍生的铜氮掺杂碳复合材料：N型和铜对选择性CO ₂电还原的协同作用 †
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2019-09-03 , DOI: 10.1039/c9cy01131e
Yuan-Sheng Cheng _{1,

2,

3,

4,

5} , Xin-Ping Chu _{1,

2,

3,

4,

5} , Min Ling _{6,

7,

8,

9,

10} , Na Li _{6,

7,

8,

9,

10} , Kong-Lin Wu _{6,

7,

8,

9,

10} , Fang-Hui Wu _{1,

2,

3,

4,

5} , Hong Li _{1,

2,

3,

4,

5} , Guozan Yuan _{1,

2,

3,

4,

5} , Xian-Wen Wei _{1,

2,

3,

4,

5}

Affiliation

铜基复合电催化剂的开发可以轻松实现高活性和选择性，以将CO ₂还原为多碳烃。探索铜与其他材料之间的协同作用可能有助于设计高效催化剂。通过比较CO ₂还原反应（CO ₂通过煅烧含N的苯并咪唑改性的Cu-BTC（1,3,5-苯三甲酸）MOF（BEN-Cu-BTC）获得的MOF衍生的铜@氮掺杂碳（Cu-NC）催化剂的RR）性能）在不同的温度下。不同类型的Cu–NC样品显示出高选择性电还原CO ₂到C ₂产物的N物种和含量依赖的催化作用。表征和实验结果表明，在400°C的退火温度下形成的高含量的吡咯N和Cu–N物种可以促进Cu表面上C ₂生成，反应速率和法拉第效率（FEs）），对于乙烯和乙醇为r_乙烯= 5.38μmolm ^-2s ^-1（FE = 11.2％）和r_乙醇= 8.83μmolm ^-2 s ^-1（FE = 18.4％）在-1.01 V下（相对于可逆氢电极（RHE））。但是，铜表面上过量的石墨氮和氧化氮会导致大量的H ₂析出并迅速降低CO _2。RR活动。这些可能是由于影响Cu-NC相互作用的吸附态和价态不同而引起的。这些结果表明，MOF衍生的Cu–NC催化剂的催化活性可以由在相应退火温度下占优势的N型物质控制，这为设计高选择性复合催化剂提供了新的思路，因为Cu–NC的电催化性能NC催化剂在8小时内保持稳定。

"点击查看英文标题和摘要"

An MOF-derived copper@nitrogen-doped carbon composite: the synergistic effects of N-types and copper on selective CO2 electroreduction†

The development of Cu-based complex electrocatalysts can lead to the facile realization of high activity and selectivity for reducing CO₂ to multi-carbon hydrocarbons; exploring the synergistic effect between Cu and other materials may help in designing highly efficient catalysts. This paper reports an impact factor for synergistic effects between Cu and nitrogen-doped carbon (NC) supports by comparing CO₂ reduction reaction (CO₂RR) performances on MOF-derived copper@nitrogen-doped carbon (Cu–NC) catalysts obtained by the calcination of N-containing benzimidazole-modified Cu-BTC (1,3,5-benzenetricarboxylic acid) MOFs (BEN-Cu-BTC) at different temperatures. Different types of Cu–NC samples show the N species- and content-dependent catalysis for the highly selective electroreduction of CO₂ to C₂ products. The characterization and experimental results indicate that the high contents of pyrrolic-N and Cu–N species formed at the annealing temperature of 400 °C can facilitate the C₂-product generation on a Cu surface, with the reaction rates and Faradaic efficiencies (FEs) for ethylene and ethanol being r_ethylene = 5.38 μmol m⁻² s⁻¹ (FE = 11.2%) and r_ethanol = 8.83 μmol m⁻² s⁻¹ (FE = 18.4%) at −1.01 V (vs. reversible hydrogen electrode (RHE)), respectively. However, excess graphitic-N and oxidized-N on the Cu surface result in considerable H₂ evolution and a rapid decrease in the CO₂RR activity. These may occur due to the differences in the adsorption and valence state affecting the Cu–NC interactions. These results indicate that the catalytic activity on MOF-derived Cu–NC catalysts can be controlled by the N-type species that dominates at the corresponding annealing temperature, offering a new tack for designing highly selective complex catalysts since the electrocatalytic performance of the Cu–NC catalysts remains stable over 8 h.

更新日期：2019-10-14

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