Citation: Tingting Zhang, Yin Wang, Xiangyang Li, Quan Zhuang, Zixuan Zhang, Hong Zhou, Qin Ding, Yingqi Wang, Yuxin Dang, Limei Duan, Jinghai Liu. Charge state modulation on boron site by carbon and nitrogen localized bonding microenvironment for two-electron electrocatalytic H₂O₂ production[J]. Chinese Chemical Letters, ;2023, 34(5): 107596. doi: 10.1016/j.cclet.2022.06.019 shu

Charge state modulation on boron site by carbon and nitrogen localized bonding microenvironment for two-electron electrocatalytic H₂O₂ production

Tingting Zhang ^{a, 1} ,
Yin Wang ^{a, 1, *,} ,
Xiangyang Li ^a ,
Quan Zhuang ^{a, *,} ,
Zixuan Zhang ^a ,
Hong Zhou ^a ,
Qin Ding ^a ,
Yingqi Wang ^b ,
Yuxin Dang ^a ,
Limei Duan ^{a, *,} ,
Jinghai Liu ^{a, *,}

a.
Inner Mongolia Key Laboratory of Carbon Nanomaterials, College of Chemistry and Materials Science, Nano Innovation Institute, Inner Mongolia Minzu University, Tongliao 028000, China
b.
Tongliao Center for Disease Control and Prevention, Tongliao 028000, China

wy19890703@126.com

zhuangquan21@outlook.com

duanlmxie@126.com

jhliu2008@sinano.ac.cn

Received Date: 28 January 2022
Revised Date: 13 May 2022
Accepted Date: 8 June 2022
Available Online: 13 June 2022

Figures(5)

Design of electrochemical active boron (B) site at solid materials to understand the relationships between the localized structure, charge state at the B site and electrocatalytic activity plays a crucial role in boosting the green electrochemical synthesis of hydrogen peroxide (H₂O₂) via two-electron oxygen reduction (2eORR) pathway. Herein, we demonstrate a carbon (C) and nitrogen (N) localized bonding microenvironment to modulate the charge state of B site at the boron-carbon nitride solid (BCNs) to realize the efficient selective electrocatalytic H₂O₂ production. The localized chemical structure of N-B-N, N-B-C and C-B-C bonds at B site can be regulated through solid-state reaction between boron nitride (BN) and porous carbon (C) at variable temperatures. The optimized BCN-1100 achieves an outstanding H₂O₂ selectivity of 89% and electron transfer number of 2.2 (at 0.55 V vs. RHE), with the production of 10.55 mmol/L during 2.5 h and the catalytic stability duration for 15000 cycles. Further first-principles calculations identified the dependency of localized bonding microenvironment on the OOH^* adsorption energies and relevant charge states at the boron site. The localized structure of B site with BNC₂-Gr configuration is predicted to be the highest 2eORR activity.
- Solid boron site,
- Charge state modulation,
- Localized bonding microenvironment,
- Two-electron oxygen reduction,
- H₂O₂ electrosynthesis
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Charge state modulation on boron site by carbon and nitrogen localized bonding microenvironment for two-electron electrocatalytic H2O2 production

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通讯作者: 陈斌, bchen63@163.com

Charge state modulation on boron site by carbon and nitrogen localized bonding microenvironment for two-electron electrocatalytic H₂O₂ production