Synergistic reduction of U(VI) and selective oxidation of benzyl alcohol to prepare benzaldehyde via WOx/g-C3N4

被引:61
作者
He, Feng [1 ,2 ]
Xiao, Qianxiang [2 ]
Chen, Yin [2 ]
Wang, Hongqing [2 ]
Wang, Xiangke [3 ]
机构
[1] Univ South China, Sch Nucl Sci & Technol, Hengyang 421001, Hunan, Peoples R China
[2] Univ South China, Sch Chem & Chem Engn, Hunan Key Lab Design & Applicat Actinide Complexes, Hengyang 421001, Hunan, Peoples R China
[3] North China Elect Power Univ, Coll Environm Sci & Engn, Beijing 102206, Peoples R China
来源
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2024年 / 343卷
基金
中国国家自然科学基金;
关键词
Photocatalysis; U(VI) reduction; Benzyl alcohol; Selective oxidation; GRAPHITIC CARBON NITRIDE; VISIBLE-LIGHT; PHOTOCATALYST; HETEROJUNCTION; SEMICONDUCTORS; PHOTOREDUCTION; ELIMINATION; SYSTEM; ENERGY; CO2;
D O I
10.1016/j.apcatb.2023.123525
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
In the photoreduction of U(VI), protective gases and additional sacrificial agents are still the major obstacles. Herein, we developed an oxygen-deficient WOx/g-C3N4 catalyst for the simultaneous reduction of U(VI) and preparation of benzaldehyde by selective oxidation of benzyl alcohol without protective gases and sacrificial agents. The removal of U(VI) by WOx/g-C3N4 could reach 98.5% and the conversion of benzyl alcohol was nearly 32% with a selectivity close to 100%. Compared with single g-C3N4 and defect-free WO3, the photoreduction activity of WOx/g-C3N4 was 10.4 and 7 times higher, respectively. Besides, the role of oxygen and oxygen defects was explored. Owing to oxygen defects in the catalyst, oxygen was adsorbed on the oxidation end (WOx) of the catalyst and activated without entering the reduction end to interfere with the photoreduction of U(VI), while favoring the generation of center dot O2- to improve the selectivity of benzaldehyde. Finally, a new mechanism was proposed.
引用
收藏
页数:13
相关论文
共 62 条
[1]   Defect engineering in photocatalytic materials [J].
Bai, Song ;
Zhang, Ning ;
Gao, Chao ;
Xiong, Yujie .
NANO ENERGY, 2018, 53 :296-336
[2]   PROJECTOR AUGMENTED-WAVE METHOD [J].
BLOCHL, PE .
PHYSICAL REVIEW B, 1994, 50 (24) :17953-17979
[3]   Ionothermal Synthesis of Crystalline, Condensed, Graphitic Carbon Nitride [J].
Bojdys, Michael J. ;
Mueller, Jens-Oliver ;
Antonietti, Markus ;
Thomas, Arne .
CHEMISTRY-A EUROPEAN JOURNAL, 2008, 14 (27) :8177-8182
[4]   A novel strategy for loading metal cocatalysts onto hollow nano-TiO2 inner surface with highly enhanced H2 production activity [J].
Chen, Nan ;
Zhou, Yu ;
Cao, Songtao ;
Wang, Ruixin ;
Jiao, Weizhou .
GREEN ENERGY & ENVIRONMENT, 2023, 8 (02) :509-518
[5]   Engineering surface oxygen defects on tungsten oxide to boost photocatalytic oxygen evolution from water splitting [J].
Chew, Yi-Hao ;
Tang, Jie-Yinn ;
Tan, Li-Jie ;
Choi, Bryan Wei Jian ;
Tan, Lling-Lling ;
Chai, Siang-Piao .
CHEMICAL COMMUNICATIONS, 2019, 55 (44) :6265-6268
[6]   Fabrication of g-C3N4/Sn3O4/Ni electrode for highly efficient photoelectrocatalytic reduction of U(VI) [J].
Dai, Zhongran ;
Lian, Junjie ;
Sun, Yusu ;
Li, Le ;
Zhang, Hui ;
Hu, Nan ;
Ding, Dexin .
CHEMICAL ENGINEERING JOURNAL, 2022, 433
[7]   Efficient Photocatalytic Extraction of Uranium over Ethylenediamine Capped Cadmium Sulfide Telluride Nanobelts [J].
Dong, Changxue ;
Qiao, Tiantao ;
Huang, Yubin ;
Yuan, Xin ;
Lian, Jie ;
Duan, Tao ;
Zhu, Wenkun ;
He, Rong .
ACS APPLIED MATERIALS & INTERFACES, 2021, 13 (10) :11968-11976
[8]   Ultrathin 2D/2D WO3/g-C3N4 step-scheme H2-production photocatalyst [J].
Fu, Junwei ;
Xu, Quanlong ;
Low, Jingxiang ;
Jiang, Chuanjia ;
Yu, Jiaguo .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2019, 243 :556-565
[9]   Effect of the Damping Function in Dispersion Corrected Density Functional Theory [J].
Grimme, Stefan ;
Ehrlich, Stephan ;
Goerigk, Lars .
JOURNAL OF COMPUTATIONAL CHEMISTRY, 2011, 32 (07) :1456-1465
[10]   A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu [J].
Grimme, Stefan ;
Antony, Jens ;
Ehrlich, Stephan ;
Krieg, Helge .
JOURNAL OF CHEMICAL PHYSICS, 2010, 132 (15)