Tuning the Electrocatalytic Properties of Black and Gray Arsenene by Introducing Heteroatoms

Sengpajan Santisouk; Phoxay Sengdala; Xingxing Jiang; Xiong-Xiong Xue; Ke-Qiu Chen; Yexin Feng

doi:10.1021/acsomega.1c00908

Tuning the Electrocatalytic Properties of Black and Gray Arsenene by Introducing Heteroatoms

ACS Omega. 2021 May 11;6(20):13124-13133. doi: 10.1021/acsomega.1c00908. eCollection 2021 May 25.

Authors

Sengpajan Santisouk¹, Phoxay Sengdala¹, Xingxing Jiang¹, Xiong-Xiong Xue², Ke-Qiu Chen¹, Yexin Feng¹

Affiliations

¹ Hunan Provincial Key Laboratory of Low-Dimensional Structural Physics & Devices, School of Physics and Electronics, Hunan University, Changsha 410082, China.
² School of Physics and Optoelectronics, Xiangtan University, Xiangtan 411105, China.

Abstract

On the basis of density functional theory calculations, we explored the catalytic properties of various heteroatom-doped black and gray arsenene toward the oxygen reduction reaction (ORR), the oxygen evolution reaction (OER), and the hydrogen evolution reaction (HER). The calculation results show that pristine black (b-As) and gray arsenene (g-As) exhibit poor catalytic performance because of too weak intermediate adsorption. Heteroatom doping plays a key role in optimizing catalytic performance. Among the candidate dopants O, C, P, S, and Sb, O is the most promising one used in arsenene to improve the ORR and OER catalytic performance. Embedding O atoms could widely tune the binding strength of reactive intermediates and improve the catalytic activity. Single O-doped g-As_O ¹ can achieve efficient bifunctional activity for both the OER and the ORR with optimal potential gap. b-As_O ¹ and b-As_O ² exhibit the optimal OER and ORR catalytic performance, respectively. For the HER, double C-doped g-As_C ² could tune the adsorption of hydrogen to an optimal value and significantly enhance the catalytic performance. These findings indicate that arsenene could provide a new platform to explore high-efficiency electrocatalysts.