Asymmetric Electron Redistribution in Niobic-Oxygen Vacancy Associates to Tune Noncovalent Interaction in CO2 Photoreduction

被引：52

作者：

Di, Jun ^{[1
]}

Chen, Chao ^{[2
,3
]}

Wu, Yao ^{[2
]}

Chen, Hao ^{[4
]}

Xiong, Jun ^{[5
]}

Long, Ran ^{[4
]}

Li, Shuzhou ^{[2
]}

Song, Li ^{[4
]}

Jiang, Wei ^{[1
]}

Liu, Zheng ^{[2
]}

机构：

[1] Nanjing Univ Sci & Technol, Natl Special Superfine Powder Engn Res Ctr, Sch Chem & Chem Engn, Nanjing 210094, Peoples R China

[2] Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore

[3] Xian Modern Chem Res Inst, Xian Key Lab Liquid Crystal & Organ Photovolta Mat, Xian 710065, Peoples R China

[4] Univ Sci & Technol China, Sch Chem & Mat Sci, Natl Synchrotron Radiat Lab, State Key Lab Particle Detect & Elect, Hefei 230026, Anhui, Peoples R China

[5] Jiangsu Univ, Inst Energy Res, Zhenjiang 212013, Peoples R China

来源：

ADVANCED MATERIALS | 2024年 / 36卷 / 25期

基金：

中国国家自然科学基金;

关键词：

asymmetric electron redistribution; Nb-O vacancy associates; noncovalent interaction; photocatalytic CO2 reduction; IONIC LIQUID;

D O I：

10.1002/adma.202401914

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The role of vacancy associates in photocatalytic CO2 reduction is an open question. Herein, the Nb-O vacancy associates (VNb-O) are engineered into niobic acid (NA) atomic layers to tailor the CO2 photoreduction performance. The intrinsic charge compensation from O to Nb around Nb-O vacancy associates can manipulate the active electronic states, leading to the asymmetric electron redistribution. These local symmetry breaking sites show a charge density gradient, forming a localized polarization field to polarize nonpolar CO2 molecules and tune the noncovalent interaction of reaction intermediates. This unique configuration contributes to the 9.3 times increased activity for photocatalytic CO2 reduction. Meantime, this VNb-O NA also shows excellent photocatalytic activity for NO3--NH4+ synthesis, with NH4+ formation rate up to 3442 mu mol g(-1) h(-1). This work supplies fresh insights into the vacancy associate design for electron redistribution and noncovalent interaction tuning in photocatalysis.

引用

页数：8

共 25 条

[1] Defect Chemistry in 2D Atomic Layers for Energy Photocatalysis [J].

Di, Jun ;

Hao, Gazi ;

Jiang, Wei ;

Liu, Zheng .

ACCOUNTS OF MATERIALS RESEARCH, 2023, 4 (11) :910-924

[2] Defective materials for CO2 photoreduction: From C1 to C2+products [J].

Di, Jun ;

Hao, Gazi ;

Liu, Guigao ;

Zhou, Jiadong ;

Jiang, Wei ;

Liu, Zheng .

COORDINATION CHEMISTRY REVIEWS, 2023, 482

[3] Polarized Cu-Bi Site Pairs for Non-Covalent to Covalent Interaction Tuning toward N2 Photoreduction [J].

Di, Jun ;

Chen, Chao ;

Wu, Yao ;

Zhao, Yunxuan ;

Zhu, Chao ;

Zhang, Yi ;

Wang, Changda ;

Chen, Hailong ;

Xiong, Jun ;

Xu, Manzhang ;

Xia, Jiexiang ;

Zhou, Jiadong ;

Weng, Yuxiang ;

Song, Li ;

Li, Shuzhou ;

Jiang, Wei ;

Liu, Zheng .

ADVANCED MATERIALS, 2022, 34 (37)

[4] Surface Local Polarization Induced by Bismuth-Oxygen Vacancy Pairs Tuning Non-Covalent Interaction for CO2 Photoreduction [J].

Di, Jun ;

Chen, Chao ;

Zhu, Chao ;

Long, Ran ;

Chen, Hailong ;

Cao, Xingzhong ;

Xiong, Jun ;

Weng, Yuxiang ;

Song, Li ;

Li, Shuzhou ;

Li, Huaming ;

Xiong, Yujie ;

Liu, Zheng .

ADVANCED ENERGY MATERIALS, 2021, 11 (41)

[5] Ultrahigh Photocatalytic CO2 Reduction Efficiency and Selectivity Manipulation by Single-Tungsten-Atom Oxide at the Atomic Step of TiO2 [J].

Feng, Yibo ;

Wang, Cong ;

Cui, Peixin ;

Li, Chong ;

Zhang, Bin ;

Gan, Liyong ;

Zhang, Shengbai ;

Zhang, Xiaoxian ;

Zhou, Xiaoyuan ;

Sun, Zhiming ;

Wang, Kaiwen ;

Duan, Youyu ;

Li, Hui ;

Zhou, Kai ;

Huang, Hongwei ;

Li, Ang ;

Zhuang, Chunqiang ;

Wang, Lihua ;

Zhang, Ze ;

Han, Xiaodong .

ADVANCED MATERIALS, 2022, 34 (17)

[6] Vacancy-defect modulated pathway of photoreduction of CO2 on single atomically thin AgInP2S6 sheets into olefiant gas [J].

Gao, Wa ;

Li, Shi ;

He, Huichao ;

Li, Xiaoning ;

Cheng, Zhenxiang ;

Yang, Yong ;

Wang, Jinlan ;

Shen, Qing ;

Wang, Xiaoyong ;

Xiong, Yujie ;

Zhou, Yong ;

Zou, Zhigang .

NATURE COMMUNICATIONS, 2021, 12 (01)

[7] Single Nb atom modified anatase TiO2(110) for efficient electrocatalytic nitrogen reduction reaction [J].

Gao, Yunnan ;

Yang, Yang ;

Hao, Leiduan ;

Hong, Song ;

Tan, Xinyi ;

Wu, Tai-Sing ;

Soo, Yun-Liang ;

Robertson, Alex W. ;

Yang, Qi ;

Sun, Zhenyu .

CHEM CATALYSIS, 2022, 2 (09) :2275-2288

[8] Amorphizing noble metal chalcogenide catalysts at the single-layer limit towards hydrogen production [J].

He, Yongmin ;

Liu, Liren ;

Zhu, Chao ;

Guo, Shasha ;

Golani, Prafful ;

Koo, Bonhyeong ;

Tang, Pengyi ;

Zhao, Zhiqiang ;

Xu, Manzhang ;

Yu, Peng ;

Zhou, Xin ;

Gao, Caitian ;

Wang, Xuewen ;

Shi, Zude ;

Zheng, Lu ;

Yang, Jiefu ;

Shin, Byungha ;

Arbiol, Jordi ;

Duan, Huigao ;

Du, Yonghua ;

Heggen, Marc ;

Dunin-Borkowski, Rafal E. ;

Guo, Wanlin ;

Wang, Qi Jie ;

Zhang, Zhuhua ;

Liu, Zheng .

NATURE CATALYSIS, 2022, 5 (03) :212-221

[9] A Multidimensional Approach to Modulating Ionizable Lipids for High-Performing and Organ-Selective mRNA Delivery [J].

He, Zepeng ;

Le, Zhicheng ;

Shi, Yi ;

Liu, Lixin ;

Liu, Zhijia ;

Chen, Yongming .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2023, 62 (43)

[10] Filling metal-organic framework mesopores with TiO2for CO2photoreduction [J].

Jiang, Zhuo ;

Xu, Xiaohui ;

Ma, Yanhang ;

Cho, Hae Sung ;

Ding, Deng ;

Wang, Chao ;

Wu, Jie ;

Oleynikov, Peter ;

Jia, Mei ;

Cheng, Jun ;

Zhou, Yi ;

Terasaki, Osamu ;

Peng, Tianyou ;

Zan, Ling ;

Deng, Hexiang .

NATURE, 2020, 586 (7830) :549-+

← 1 2 3 →