Enhanced photocatalytic N2 fixation via defective and fluoride modified TiO2 surface

被引:182
作者
Guan, Renquan [1 ,2 ]
Wang, Dandan [1 ]
Zhang, Yujun [3 ]
Liu, Chen [3 ]
Xu, Wei [3 ]
Wang, Jiaou [3 ]
Zhao, Zhao [1 ,2 ]
Feng, Ming [1 ]
Shang, Qingkun [2 ]
Sun, Zaicheng [4 ]
机构
[1] Jilin Normal Univ, Key Lab Funct Mat Phys & Chem, Minist Educ, Key Lab Preparat & Applicat Environm Friendly Mat, Changchun 130103, Peoples R China
[2] Northeast Normal Univ, Fac Chem, Changchun 130103, Peoples R China
[3] Chinese Acad Sci, Inst High Energy Phys, Yuquan Rd 19B, Beijing 100049, Peoples R China
[4] Beijing Univ Technol, Coll Environm & Energy Engn, Dept Chem & Chem Engn, Ctr Excellence Environm Safety & Biol Effects,Bei, 100 Pingleyuan, Beijing 100124, Peoples R China
基金
中国国家自然科学基金;
关键词
TiO2; Photocatalysis Oxygen vacancy; N-2; fixation; Hydrophobized; OXYGEN VACANCIES; S-VACANCIES; NITROGEN; REDUCTION; AMMONIA; WATER; PHOTOFIXATION; PERFORMANCE; NANOSHEETS; NH3;
D O I
10.1016/j.apcatb.2020.119580
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
Photocatalytic N-2 fixation (PNF) provides a low-cost route to generate ammonia. The poor conversion efficiency from photon to ammonia seriously hinders the step forward because of the low concentration of N-2 molecules. Herein, we demonstrate a photocatalyst with surface oxygen vacancies (Vo) and a F modified surface to facilitate N-2 adsorption and activation on the surface of catalysts. The Vo site promotes the chemical adsorption of N-2, electron transfer from catalyst to N-2. F modification switches the TiO2 surface properties from hydrophilic to aerophilic, thus facilitating the adsorption of N-2. Meanwhile, the hydrogen reduction reaction (HER) is sup-pressed, as protons hard to adsorb on F capped surfaces. The optimal NH3 production rate can reach 206 mu molh(-1)g(-1), which is similar to 9 times higher than that of pure TiO2 nanoparticles (similar to 23 mu molh(-1)g(-1)). This report provides a potential strategy to overcome mass transfer limitation and achieve a high conversion efficiency in PNF.
引用
收藏
页数:10
相关论文
共 57 条
[1]   Hierarchical hollow nanotubes of NiFeV-layered double hydroxides@CoVP heterostructures towards efficient, pH-universal electrocatalytical nitrogen reduction reaction to ammonia [J].
Arif, Muhammad ;
Yasin, Ghulam ;
Luo, Lan ;
Ye, Wen ;
Mushtaq, Muhammad Asim ;
Fang, Xiaoyu ;
Xiang, Xu ;
Ji, Shengfu ;
Yan, Dongpeng .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2020, 265
[2]  
Borman STU, 2016, CHEM ENG NEWS, V94, P9
[3]   Constraints on superconducting cosmic strings from the global 21-cm signal before reionization [J].
Brandenberger, Robert ;
Cyr, Bryce ;
Shi, Rui .
JOURNAL OF COSMOLOGY AND ASTROPARTICLE PHYSICS, 2019, (09)
[4]   XAFS studies of surface structures of TiO2 nanoparticles and photocatalytic reduction of metal ions [J].
Chen, LX ;
Rajh, T ;
Wang, ZY ;
Thurnauer, MC .
JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (50) :10688-10697
[5]   Mo-doped SnS2 with enriched S-vacancies for highly efficient electrocatalytic N2 reduction: the critical role of the Mo-Sn-Sn trimer [J].
Chu, Ke ;
Wang, Jing ;
Liu, Ya-ping ;
Li, Qing-qing ;
Guo, Ya-li .
JOURNAL OF MATERIALS CHEMISTRY A, 2020, 8 (15) :7117-7124
[6]   Fe-doping induced morphological changes, oxygen vacancies and Ce3+-Ce3+ pairs in CeO2 for promoting electrocatalytic nitrogen fixation [J].
Chu, Ke ;
Cheng, Yong-hua ;
Li, Qing-qing ;
Liu, Ya-ping ;
Tian, Ye .
JOURNAL OF MATERIALS CHEMISTRY A, 2020, 8 (12) :5865-5873
[7]   Synergistic boron-dopants and boron-induced oxygen vacancies in MnO2 nanosheets to promote electrocatalytic nitrogen reduction [J].
Chu, Ke ;
Liu, Ya-ping ;
Cheng, Yong-hua ;
Li, Qing-qing .
JOURNAL OF MATERIALS CHEMISTRY A, 2020, 8 (10) :5200-5208
[8]   Filling the nitrogen vacancies with sulphur dopants in graphitic C3N4 for efficient and robust electrocatalytic nitrogen reduction [J].
Chu, Ke ;
Li, Qing-qing ;
Liu, Ya-ping ;
Wang, Jing ;
Cheng, Yong-hua .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2020, 267
[9]   Multi-functional Mo-doping in MnO2 nanoflowers toward efficient and robust electrocatalytic nitrogen fixation [J].
Chu, Ke ;
Liu, Ya-ping ;
Li, Yu-biao ;
Guo, Ya-li ;
Tian, Ye ;
Zhang, Hu .
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY, 2020, 264
[10]   Functional Single-Cell Approach to Probing Nitrogen-Fixing Bacteria in Soil Communities by Resonance Raman Spectroscopy with 15N2 Labeling [J].
Cui, Li ;
Yang, Kai ;
Li, Hong-Zhe ;
Zhang, Han ;
Su, Jian-Qiang ;
Paraskevaidi, Maria ;
Martin, Francis L. ;
Ren, Bin ;
Zhu, Yong-Guan .
ANALYTICAL CHEMISTRY, 2018, 90 (08) :5082-5089