Wang Nan, Mei Riguo, Zhang Guobin, Chen Liqiong, Yang Tao, Chen Zhongwei, Lin Xidong, Liu Qingxia
College of Applied Sciences, Shenzhen University, Shenzhen 518060, P. R. China.
Future Technology School, Shenzhen Technology University, Shenzhen 518118, P. R. China.
ACS Appl Mater Interfaces. 2024 Aug 14;16(32):42128-42137. doi: 10.1021/acsami.4c06157. Epub 2024 Jul 30.
The electrochemical CO reduction reaction (CORR) into high-value carbon compounds such as CO and HCOOH is a promising strategy for the utilization and conversion of emitted CO. However, the selectivity of the CORR for HCOOH is typically less than 90% and operates within a narrow voltage range, which limits its practical application. Herein, we propose a novel heterostructural aerogel as a highly efficient electrocatalyst for CORR to HCOOH. This catalyst consists of Cu-Sn-O solid solutions embedded in a reduced graphene oxide matrix (Cu-Sn-O/rGO). The incorporation of Cu into the SnO matrix enhances HCOOH production by improving the adsorption of the *OCHO intermediate and inhibiting H evolution, as confirmed by measurements and computational studies. As a result, Cu-Sn-O/rGO achieves a remarkable Faradaic efficiency (FE) of up to 91.4% for HCOOH and maintains high selectivity over a broad operating voltage range (-0.8 to -1.1 V). Additionally, the assembled Zn-CO batteries demonstrated an excellent power density of 1.14 mW/cm and exceptional stability for over 25 h.
将电化学CO还原反应（CORR）转化为诸如CO和HCOOH等高价值碳化合物是一种有前景的排放CO利用和转化策略。然而，CORR对HCOOH的选择性通常低于90%，且在狭窄的电压范围内运行，这限制了其实际应用。在此，我们提出一种新型异质结构气凝胶作为用于CORR生成HCOOH的高效电催化剂。该催化剂由嵌入还原氧化石墨烯基质（Cu-Sn-O/rGO）中的Cu-Sn-O固溶体组成。正如测量和计算研究所证实的，将Cu掺入SnO基质中通过改善*OCHO中间体的吸附和抑制H析出提高了HCOOH的产量。结果，Cu-Sn-O/rGO对HCOOH实现了高达91.4%的显著法拉第效率（FE），并在宽工作电压范围（-0.8至-1.1 V）内保持高选择性。此外，组装的Zn-CO电池表现出1.14 mW/cm的优异功率密度和超过25小时的出色稳定性。
