Iridium single-atom catalyst on nitrogen-doped carbon for formic acid oxidation synthesized using a general host–guest strategy

• Published in: Nature chemistry Vol. 12; no. 8; pp. 764 - 772
• Main Authors: Li, Zhi, Chen, Yuanjun, Ji, Shufang, Tang, Yan, Chen, Wenxing, Li, Ang, Zhao, Jie, Xiong, Yu, Wu, Yuen, Gong, Yue, Yao, Tao, Liu, Wei, Zheng, Lirong, Dong, Juncai, Wang, Yu, Zhuang, Zhongbin, Xing, Wei, He, Chun-Ting, Peng, Chao, Cheong, Weng-Chon, Li, Qiheng, Zhang, Maolin, Chen, Zheng, Fu, Ninghua, Gao, Xin, Zhu, Wei, Wan, Jiawei, Zhang, Jian, Gu, Lin, Wei, Shiqiang, Hu, Peijun, Luo, Jun, Li, Jun, Chen, Chen, Peng, Qing, Duan, Xiangfeng, Huang, Yu, Chen, Xiao-Ming, Wang, Dingsheng, Li, Yadong
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 01.08.2020; Nature Publishing Group
• Subjects: 639/638/161/886; 639/638/298; 639/638/77/886; Analytical Chemistry; Atom economy; Biochemistry; Carbon; Carbon monoxide; Carbon monoxide poisoning; Catalysts; Chemistry; Chemistry and Materials Science; Chemistry/Food Science; Copper; Density functional theory; Displays; Electronic structure; Equivalence; First principles; Formic acid; Inorganic Chemistry; Iridium; Manganese; Molybdenum; Nanoparticles; Nickel; Nitrogen; Organic Chemistry; Oxidation; Palladium; Physical Chemistry; Platinum; Poisoning; Properties (attributes); Single atom catalysts; Strategy
• ISSN: 1755-4330; 1755-4349; 1755-4349
• DOI: 10.1038/s41557-020-0473-9

Single-atom catalysts not only maximize metal atom efficiency, they also display properties that are considerably different to their more conventional nanoparticle equivalents, making them a promising family of materials to investigate. Herein we developed a general host–guest strategy to fabricate various metal single-atom catalysts on nitrogen-doped carbon (M 1 /CN, M = Pt, Ir, Pd, Ru, Mo, Ga, Cu, Ni, Mn). The iridium variant Ir 1 /CN electrocatalyses the formic acid oxidation reaction with a mass activity of 12.9  A mg Ir − 1 whereas an Ir/C nanoparticle catalyst is almost inert (~4.8 × 10 −3   A mg Ir − 1 ). The activity of Ir 1 /CN is also 16 and 19 times greater than those of Pd/C and Pt/C, respectively. Furthermore, Ir 1 /CN displays high tolerance to CO poisoning. First-principle density functional theory reveals that the properties of Ir 1 /CN stem from the spatial isolation of iridium sites and from the modified electronic structure of iridium with respect to a conventional nanoparticle catalyst. Single-atom catalysts maximize metal atom efficiency and exhibit properties that can be considerably different to their nanoparticle equivalent. Now a general host–guest strategy to make various single-atom catalysts on nitrogen-doped carbon has been developed; the iridium variant electrocatalyses the formic acid oxidation reaction with high mass activity and displays high tolerance to CO poisoning.