State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, PR China.
Department of Materials Chemistry, School of Chemical Engineering and Materials Science, Quanzhou Normal University, Quanzhou, 362000, China.
ChemSusChem. 2018 Mar 9;11(5):881-887. doi: 10.1002/cssc.201702338. Epub 2018 Feb 15.
Cu is a unique catalyst for CO electroreduction, since it can catalyze CO reduction to a series of hydrocarbons, alcohols, and carboxylic acids. Nevertheless, such Cu catalysts suffer from poor selectivity. High pressure of CO is considered to facilitate the activity and selectivity of CO reduction. Herein, a new strategy is presented for CO reduction with improved C H selectivity on a Cu catalyst by using CO capture materials as the support at ambient pressure. N-doped carbon (N C) was synthesized through high-temperature carbonization of melamine and l-lysine. We observed that the CO uptake capacity of N C depends on both the microporous area and the content of pyridinic N species, which can be controlled by the carbonization temperature (600-800 °C). The as-prepared CuO/N C catalysts exhibit a considerably higher C H faradaic efficiency (36 %) than CuO supported on XC-72 carbon black (19 %), or unsupported CuO (20 %). Moreover, there is a good linear relationship between the C H faradaic efficiency and CO uptake capacity of the supports for CuO. The local high CO concentration near Cu catalysts, created by CO capture materials, was proposed to increase the coverage of CO intermediate, which is favorable for the coupling of two CO units in the formation of C H . This study demonstrates that pairing Cu catalysts with CO capture supports is a promising approach for designing highly effective CO reduction electrocatalysts.
铜是一种独特的 CO 电还原催化剂，因为它可以催化 CO 还原为一系列烃类、醇类和羧酸类。然而，这样的 Cu 催化剂的选择性较差。高 CO 压力被认为有利于 CO 还原的活性和选择性。在此，通过使用 CO 捕获材料作为支撑体在环境压力下，提出了一种提高 Cu 催化剂上 CO 还原的 C H 选择性的新策略。通过高温碳化三聚氰胺和 l-赖氨酸合成了掺氮碳（N C）。我们观察到，N C 的 CO 吸收能力取决于微孔面积和吡啶氮物种的含量，这可以通过碳化温度（600-800°C）来控制。所制备的 CuO/N C 催化剂的 C H 法拉第效率（36％）明显高于 CuO 负载在 XC-72 炭黑（19％）或无载体 CuO（20％）上的催化剂。此外，CuO 载体的 C H 法拉第效率与 CO 吸收能力之间存在良好的线性关系。CO 捕获材料在 Cu 催化剂附近产生的局部高 CO 浓度被认为增加了 CO 中间物的覆盖率，这有利于在 C H 的形成中两个 CO 单元的偶联。这项研究表明，将 Cu 催化剂与 CO 捕获支撑体配对是设计高效 CO 还原电催化剂的一种有前途的方法。
