General Method to Introduce Ï -Electrons into Oxygen-Doped Porous Carbon Nitride for Photocatalytic Hydrogen Evolution and Toluene Oxidation

Sun, Zongzhao1; Tan, Yueyang2; Shi, Xinkai3; Li, Bingwen4; Wang, Xinfang4; Wen, Jiangwei3; Huang, Limin2; Lau, Woon-Ming1

2024-01-03

10.1021/acssuschemeng.3c06962

ACS SUSTAINABLE CHEMISTRY & ENGINEERING   影响因子和分区

2168-0485

pi-Electrons have been successfully connected to an oxygen-doped porous carbon nitride by one-pot pyrolysis of the mixture of urea, ethanol, and 4-iodobenzaldehyde (IBD) in the atmosphere. The resulting COCN20 exhibits superior photocatalytic hydrogen production up to 6.88 mmol h(-1) g(cat)(-1) with a relatively high apparent quantum efficiency (20.6% at 325 nm) as well as toluene oxidation with an outstanding conversion rate of 3.75 mmol h(-1) g(cat)(-1) under 460 nm irradiation. Other pi-electrons from aromatic heterocycles could also be grafted to the network for the general synthesis, demonstrating higher hydrogen evolution rates (e.g., 9.32 mmol h(-1) g(cat)(-1) with the thiophene-pi-electrons coupling). The enhanced n -> pi* electron transition and activated midgap states are found to extend the light-responsive region and improve the capture of effective electrons, while the novel porous architecture encourages the efficient mass-transfer rate and improves light harvesting. This work showcases a straightforward and scalable approach to fabricate immensely proficient photocatalysts composed of porous carbon nitride. Furthermore, it opens up a novel pathway for the methodical development and production of sophisticated photocatalysts that harness the powerful synergistic effects achieved by simultaneously adjusting and refining the electronic, surface, and molecular structures.

porous carbon nitride pi-electrons oxygendoping photocatalytic hydrogen evolution tolueneoxidation

SCI ; EI

英语

通讯

Natural Science Foundation of Shandong Province[JCYJ20220818100212027] ; Shenzhen Science and Technology Innovation Commission["ZR2021QB159","ZR2020QB130"] ; Natural Science Foundation of Shandong Province[21902083] ; National Natural Science Foundation of China[2021xjrc102]

Chemistry ; Science & Technology - Other Topics ; Engineering

Chemistry, Multidisciplinary ; Green & Sustainable Science & Technology ; Engineering, Chemical

WOS:001143577900001

AMER CHEMICAL SOC

Web of Science

1.Linyi Univ, Coll Chem & Chem Engn, Linyi 276000, Shandong, Peoples R China
2.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China
3.Qufu Normal Univ, Inst Med & Mat Appl Technol, Coll Chem & Chem Engn, Qufu 273165, Shandong, Peoples R China
4.Dezhou Univ, Inst Biophys, Shandong Key Lab Biophys, Coll Chem & Chem Engn, Dezhou 253023, Shandong, Peoples R China

Sun, Zongzhao,Tan, Yueyang,Shi, Xinkai,et al. General Method to Introduce Ï -Electrons into Oxygen-Doped Porous Carbon Nitride for Photocatalytic Hydrogen Evolution and Toluene Oxidation[J]. ACS SUSTAINABLE CHEMISTRY & ENGINEERING,2024,12(2).

Sun, Zongzhao.,Tan, Yueyang.,Shi, Xinkai.,Li, Bingwen.,Wang, Xinfang.,...&Lau, Woon-Ming.(2024).General Method to Introduce Ï -Electrons into Oxygen-Doped Porous Carbon Nitride for Photocatalytic Hydrogen Evolution and Toluene Oxidation.ACS SUSTAINABLE CHEMISTRY & ENGINEERING,12(2).

Sun, Zongzhao,et al."General Method to Introduce Ï -Electrons into Oxygen-Doped Porous Carbon Nitride for Photocatalytic Hydrogen Evolution and Toluene Oxidation".ACS SUSTAINABLE CHEMISTRY & ENGINEERING 12.2(2024).