Lewis functional nanodiamonds for efficient metal-free photocatalytic CO₂ reduction

Gao, Xiaowu1,2; Han, Xinyue1; Zhao, Ziwei1,2; Huang, Ning-Yu3; Jiao, Keran1,4; Song, Pengfei5; Zhu, Jiaqi2; Wang, Yongjie1,2

2024-06-01

10.1039/d4ta02877e

JOURNAL OF MATERIALS CHEMISTRY A   影响因子和分区

2050-7488

2050-7496

Artificial photosynthesis of fuels and valuable compounds from CO2 and H2O, as a flawless method, has aroused universal interest. Metal-free catalytic materials with balanced efficiency and stability have rarely been demonstrated. To date, emerging carbon-based photocatalysts promise to break the ordeal of extreme environments for catalysts, leading to practical industrial applications. Among them, surface functional group-modified nanodiamonds offer additional possibilities in terms of long-term stability and tunable catalytic activity. In this work, the nature of distinctions in photocatalytic efficacy induced by two varieties of NDs modified with distinct Lewis acid-base functional groups was also systematically investigated. Furthermore, by using a bottom-up approach, the three-dimensional g-C3N4 (3D CN) loaded with nanodiamond (ND) functionalized with amino and carboxyl groups, has been demonstrated as an impressive metal-free photocatalyst for photosynthetic production of CO. Combining in situ photoelectrochemical analysis and density functional theory, the mechanism of heterojunction formation between 3D CN and NDs modified with different functional groups was elucidated from kinetic and thermodynamic perspectives. The synergistic CO production rate of amino-modified NDs was found to be roughly 1.97 times higher than that of carboxyl-modified NDs. This pioneering work introduces promising sp(3)-hybridized ND materials into photoreduction CO2 systems in terms of surface chemistry, helping to establish an improved understanding of this emerging carbon material.

SCI ; EI

英语

其他

National Natural Science Foundation of China[52102162] ; Guangdong Basic and Applied Basic Research Foundation[2022A1515011794] ; Shenzhen Constantly-Supported Project for Universities and Colleges[GXWD20231130110722002]

Chemistry ; Energy & Fuels ; Materials Science

Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary

WOS:001258303500001

ROYAL SOC CHEMISTRY

Web of Science

1.Harbin Inst Technol, Sch Sci, Guangdong Prov Key Lab Semicond Optoelect Mat & In, Shenzhen 518055, Peoples R China
2.Harbin Inst Technol, Natl Key Lab Sci & Technol Adv Composites Special, Harbin 150080, Peoples R China
3.Southern Univ Sci & Technol SUSTech, SUSTech Kyoto Univ Adv Energy Mat Joint Innovat La, Dept Chem, Shenzhen Key Lab Micro Nanoporous Funct Mat SKLPM, Shenzhen 518055, Peoples R China
4.Univ Manchester, Dept Chem Engn, Oxford Rd, Manchester M13 9PL, England
5.Xian Jiaotong Liverpool Univ, Sch Adv Technol, Suzhou 215000, Peoples R China

Gao, Xiaowu,Han, Xinyue,Zhao, Ziwei,et al. Lewis functional nanodiamonds for efficient metal-free photocatalytic CO₂ reduction[J]. JOURNAL OF MATERIALS CHEMISTRY A,2024.

Gao, Xiaowu.,Han, Xinyue.,Zhao, Ziwei.,Huang, Ning-Yu.,Jiao, Keran.,...&Wang, Yongjie.(2024).Lewis functional nanodiamonds for efficient metal-free photocatalytic CO₂ reduction.JOURNAL OF MATERIALS CHEMISTRY A.

Gao, Xiaowu,et al."Lewis functional nanodiamonds for efficient metal-free photocatalytic CO₂ reduction".JOURNAL OF MATERIALS CHEMISTRY A (2024).