Fan Tingting, Zhang Jiguang, Zhang Yanping, Ma Xintao, Huang Pingping, Zhang Shuhong, Chen Zhou, Wang Miao, Dong Yunyun, Yi Xiaodong
College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, P. R. China.
College of Materials, Xiamen University, Xiamen 361005, P. R. China.
ACS Appl Mater Interfaces. 2022 Mar 16;14(10):12314-12322. doi: 10.1021/acsami.2c00133. Epub 2022 Mar 3.
The efficient electrochemical conversion of carbon dioxide (CO) to carbon monoxide (CO) using renewable energy is an effective route to pursue carbon neutrality. Optimizing the binding energy of CO on palladium (Pd) metal-based materials used in this process is to make sure the timely desorption of CO from their active sites is critical. Tuning the electronic structure of the Pd center is an effective strategy to optimize its catalytic performance. Herein, we rationally design Pd nanoparticles (NPs)/polymeric carbon nitride (CN) (Pd/CN) composite, which alters the electronic structure of Pd by introducing the interfacial polarization effect to accelerate CO desorption and improve CO selectivity of Pd catalyst. The optimized Pd/CN exhibits a CO Faradaic efficiency of 92.7% at -0.9 V reversible hydrogen electrode in CO-saturated 0.1 M KHCO solution. Experimental investigations and theoretical calculations jointly confirm that the enhanced CO selectivity and stability originate from the electron transfer at the Pd/CN interface, and the weakened *CO adsorption on the palladium hydride surface.
利用可再生能源将二氧化碳（CO₂）高效电化学转化为一氧化碳（CO）是实现碳中和的有效途径。在此过程中，优化CO在钯（Pd）基金属材料上的结合能，以确保CO能及时从其活性位点解吸至关重要。调节Pd中心的电子结构是优化其催化性能的有效策略。在此，我们合理设计了钯纳米颗粒（NPs）/聚合氮化碳（CN）（Pd/CN）复合材料，通过引入界面极化效应改变Pd的电子结构，以加速CO解吸并提高Pd催化剂对CO的选择性。优化后的Pd/CN在-0.9 V可逆氢电极下于CO饱和的0.1 M KHCO₃溶液中表现出92.7%的CO法拉第效率。实验研究和理论计算共同证实，CO选择性和稳定性的提高源于Pd/CN界面的电子转移以及*CO在氢化钯表面吸附的减弱。
