A "competitive occupancy" strategy toward Co-N-4 single-atom catalysts embedded in 2D TiN/rGO sheets for highly efficient and stable aromatic nitroreduction
Gu, Y; Wu, AP; Wang, L; Wang, DX; Yan, HJ; Yu, P; Xie, Y; Tian, CG; Sun, FF; Fu, HG
刊名JOURNAL OF MATERIALS CHEMISTRY A
2020
卷号8期号:9页码:4807-4815
关键词METAL HETEROSTRUCTURES HYDROGENATION GRAPHENE
ISSN号2050-7488
DOI10.1039/c9ta13615k
文献子类期刊论文
英文摘要Single-atom catalysts (SACs) have been promising in various catalytic fields, but the controllable synthesis of SACs with high stability remains challenging. Here, we show a robust strategy toward the fabrication of highly efficient and stable SACs based on the "competitive occupancy" of two metal (M) species on graphene oxide (GO). The abundant M-1 (Ti) species predominantly occupy more groups of GO, thereby leaving a tiny number of groups in the gaps of the M-1 species to combine with M-2 (Co2+, etc.) species. Consequently, this guarantees the formation of Co-N-4 SACs embedded in 2D TiN/rGO sheets during nitridation. Further, TiN can act as a "spacer" to prevent Co-N-4 from aggregation, thereby improving catalyst stability. Co-N-4/TiN-rGO exhibits outstanding catalytic performance for the fast conversion of highly concentrated aromatic nitro compounds (similar to 0.3-2 mM) into amino compounds and excellent recyclability, which is the best among reported catalysts. In contrast, TiN/rGO has no obvious activity, and Co4N-rGO prepared without Ti competition shows poor activity and stability, which indicates the vital role of Co-N-4 and TiN for obtaining the remarkable catalytic ability of Co-N-4/TiN-rGO. The reaction mechanism is also proposed based on theoretical calculations. The strategy can be used to design Ni (Fe, Cr, Cu)-based SACs.
语种英语
内容类型期刊论文
源URL[http://ir.sinap.ac.cn/handle/331007/32669]  
专题上海应用物理研究所_中科院上海应用物理研究所2011-2017年
作者单位1.Heilongjiang Univ, Key Lab Funct Inorgan Mat Chem, Minist Educ Peoples Republ China, Harbin 150080, Peoples R China
2.Chinese Acad Sci, Shanghai Inst Appl Phys, SSRF, Shanghai 201204, Peoples R China
3.Harbin Engn Univ, Coll Mat Sci & Chem Engn, Minist Educ, Key Lab Superlight Mat & Surface Technol, Harbin 150001, Peoples R China
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Gu, Y,Wu, AP,Wang, L,et al. A "competitive occupancy" strategy toward Co-N-4 single-atom catalysts embedded in 2D TiN/rGO sheets for highly efficient and stable aromatic nitroreduction[J]. JOURNAL OF MATERIALS CHEMISTRY A,2020,8(9):4807-4815.
APA Gu, Y.,Wu, AP.,Wang, L.,Wang, DX.,Yan, HJ.,...&Fu, HG.(2020).A "competitive occupancy" strategy toward Co-N-4 single-atom catalysts embedded in 2D TiN/rGO sheets for highly efficient and stable aromatic nitroreduction.JOURNAL OF MATERIALS CHEMISTRY A,8(9),4807-4815.
MLA Gu, Y,et al."A "competitive occupancy" strategy toward Co-N-4 single-atom catalysts embedded in 2D TiN/rGO sheets for highly efficient and stable aromatic nitroreduction".JOURNAL OF MATERIALS CHEMISTRY A 8.9(2020):4807-4815.
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