Oxygenated P/N co-doped carbon for efficient 2e- oxygen reduction to H2O2

被引:37
作者
Li, Zongge [1 ,2 ]
Kumar, Anuj [4 ]
Liu, Nianxi [1 ]
Cheng, Ming [2 ]
Zhao, Changkai [1 ]
Meng, Xiangshe [1 ]
Li, Huifang [3 ]
Zhang, Ying [2 ]
Liu, Zhiming [3 ]
Zhang, Guoxin [1 ]
Sun, Xiaoming [5 ]
机构
[1] Shandong Univ Sci & Technol, Dept Energy Storage Technol, Qingdao 266590, Shandong, Peoples R China
[2] China Univ Petr East China, State Key Lab Heavy Oil Proc, Qingdao 266580, Shandong, Peoples R China
[3] Qingdao Univ Sci & Technol, Coll Electromech Engn, Shandong Engn Lab Preparat & Applicat High Perfor, Qingdao 266061, Shandong, Peoples R China
[4] GLA Univ, Dept Chem, Mathura 281406, India
[5] Beijing Univ Chem Technol, Coll Chem, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
基金
中国国家自然科学基金;
关键词
HYDROGEN-PEROXIDE; ACTIVE-SITE; NITROGEN; ELECTROCATALYSTS; GRAPHENE; NANOCARBON; 2-ELECTRON;
D O I
10.1039/d2ta02590f
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Direct H2O2 production via the 2e(-) electrocatalytic oxygen reduction reaction (ORR) offers unique prospects for sanitization and water purification. Search for cheap, effective, selective catalysts for this process is challenging. In this work, a type of doped carbon material with rich edged P atoms co-functionalized with O and N atoms was synthesized via simple solvothermal treatment of P2O5 in formamide, followed by inert annealing. The structures and compositions of O-P/N-C materials were systematically characterized and analyzed. The optimal O-P/N-C900 sample was revealed to contain high P content (2.49 at%) and N content (11.56 at%). Electrochemical measurements revealed that the O-P/N-C900 sample achieved a very high H2O2 yield rate of 698.4 mmol g(cat.)(-1) h(-1) and a high Faradaic efficiency of 87% in a H-type cell. The density functional theory (DFT) calculations confirmed that the edged P atom with the co-functionalization of O and N atoms possessed the lowest energy barrier for promoting the selective 2e(-) ORR, showing good alignment with experiments. This work provides a new strategy for the controllable synthesis of carbon materials decorated with oxygenated heteroatom doping for electrochemical H2O2 synthesis.
引用
收藏
页码:14355 / 14363
页数:9
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