Chen Haixin, Zhang Xiaofeng, Geng Shipeng, Song Shuqin, Wang Yi
The Key Lab of Low-Carbon Chemistry and Energy Conservation of Guangdong Province, PCFM, School of Chemical Engineering and Technology, School of Materials Science and Engineering, Sun Yat-sen University, Guangzhou, 510275, China.
Small Methods. 2022 Sep;6(9):e2200636. doi: 10.1002/smtd.202200636. Epub 2022 Jul 25.
Hydrogen production from water electrolysis is important for the sustainable development of hydrogen energy. Nevertheless, the naturally torpid property of anodic oxygen evolution reaction (OER) kinetics and poor stability of its catalysts significantly restrict the development of electrochemical water splitting. Here, a Ru Cr O electrocatalyst is synthesized, which reveals excellent OER activity with the overpotential of only 195 mV at 10 mA cm and excellent stability with the potential increase of merely 5.3 mV after 20 h continuous OER test in acidic media. Theoretical calculations reveal that the solubilizing of Cr into RuO could adjust the electron distribution, making the d-band center of Ru far away from the Fermi level. This behavior reduces the binding energy with Ru and O and accelerates the rate-determining step of OER (i.e., the formation of *OOH), thereby increasing OER activity. In addition, the incorporation of Cr increases the energy of oxygen defect formation and reduces the participation of lattice oxygen, thus improving the stability of the catalyst. This research furnishes a feasible policy for the development of highly active and stable catalysts in acidic media by regulating the electronic structure of RuO .
通过水电解制氢对于氢能的可持续发展至关重要。然而,阳极析氧反应(OER)动力学的天然迟缓特性及其催化剂的稳定性差严重限制了电化学水分解的发展。在此,合成了一种RuCrO电催化剂,其在10 mA cm时过电位仅为195 mV,展现出优异的OER活性,并且在酸性介质中连续进行20小时OER测试后,电位仅增加5.3 mV,具有出色的稳定性。理论计算表明,Cr溶解到RuO中可调节电子分布,使Ru的d带中心远离费米能级。这种行为降低了与Ru和O的结合能,并加速了OER的速率决定步骤(即*OOH的形成),从而提高了OER活性。此外,Cr的掺入增加了氧缺陷形成的能量并减少了晶格氧的参与,从而提高了催化剂的稳定性。本研究通过调节RuO的电子结构,为在酸性介质中开发高活性和稳定的催化剂提供了一种可行策略。