Article
Chemistry, Multidisciplinary
Lei Wang, Bifa Ji, Yongping Zheng, Yongbing Tang
Summary: This study presents the theoretical prediction and experimental realization of an asymmetrically coordinated iridium single-atom catalyst for the formic acid oxidation reaction. Theoretical calculations show that the substitution of nitrogen with oxygen in the symmetric IrN4 motif can moderate the binding strength of key intermediates and achieve near-zero overpotential. The as-designed catalyst exhibits significantly higher mass activity compared to state-of-the-art Pd/C and Pt/C catalysts.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Materials Science, Multidisciplinary
Cheng Liu, Wei Liu, Mao-sheng Miao, Jing-yao Liu
Summary: Graphene-based carbon allotropes, particularly egg tray graphene (ETG), have been found to be effective support materials for single-atom catalysts (SACs). In this study, three N-doped ETG supported Pd SACs were designed and their catalytic performance in formic acid dehydrogenation was investigated. The results showed that Pd@ETG-N-3 exhibited the best catalytic activity, surpassing Pd(111), and the N doping in the ETG substrate greatly enhanced the activity and selectivity of the SACs.
Article
Chemistry, Multidisciplinary
Jiaping Zhu, Xuecheng Li, Xiaolin Yang, Dang Wu, Xingyuan Chen, Huakai Xu, Lijie Li, Changlin Yu, Vivek Polshettiwar, Hua Tan
Summary: In this study, nitrogen-doped carbon spheres supported single-atom Cu catalysts were prepared and applied in the oxidation of glycerol to formic acid. The catalyst exhibited unique structure, high activity and selectivity, and demonstrated good stability in consecutive catalytic runs.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Energy & Fuels
Arina N. Suboch, Olga Y. Podyacheva
Summary: Bamboo-like nitrogen-doped carbon nanotubes were utilized to synthesize supported palladium catalysts for hydrogen production via formic acid decomposition. The presence of nitrogen centers in N-CNTs plays a beneficial role in forming active isolated palladium ions and dispersed palladium nanoparticles. The activity of the catalysts is determined by the ionic capacity of N-CNTs and dispersion of metallic nanoparticles stabilized on the nitrogen centers.
Article
Chemistry, Multidisciplinary
Liu Jiao, Chenghui Mao, Fengfei Xu, Xueyi Cheng, Peixin Cui, Xizhang Wang, Lijun Yang, Qiang Wu, Zheng Hu
Summary: By constructing gold single-atom catalysts on nitrogen-doped carbon nanocages, high mass activity for electrocatalytic carbon dioxide reduction reaction to produce syngas can be achieved.
Article
Biochemistry & Molecular Biology
Gongguo Zhang, Yingying Wang, Yanyun Ma, Haifeng Zhang, Yiqun Zheng
Summary: In this study, Ir(IV)-doped PdAg alloy nanodendrites were successfully synthesized and demonstrated enhanced activity, reaction kinetics, and long-term stability as an electrocatalyst for the formic acid oxidation reaction (FAOR) in an acidic medium. The carbon-supported PdAgIr nanodendrites exhibited a prominent mass activity, surpassing that of their PdAg and Pd counterparts, as well as commercial Pt/C.
Article
Chemistry, Physical
Cheng Liu, Qiming Bing, Jing-yao Liu
Summary: In this study, the catalytic performance of nitrogen-doped graphene supported Pd-1 single-atom and Pd-4 single-cluster catalysts for dehydrogenation of formic acid was systematically studied using density functional theory calculations. The results showed that the different nitrogen dopants have different effects on the catalytic activity, with the Pd-4 single-cluster catalyst exhibiting the best catalytic performance on a specific nitrogen-doped support.
APPLIED SURFACE SCIENCE
(2022)
Article
Materials Science, Multidisciplinary
Olga Podyacheva, Arina Korobova, Svetlana Yashnik, Dmitry Svintsitskiy, Olga Stonkus, Vladimir Sobolev, Valentin Parmon
Summary: Palladium catalysts supported on nitrogen-containing carbon nanotubes showed high activity in the gas-phase formic acid decomposition for hydrogen production. The way of carbon tube doping by nitrogen greatly influenced the catalyst activity. Single-atom Pd2+ species on bamboo-like nitrogen-containing carbon nanotubes played a key role in the catalyst activity. Treating oxidized multiwalled carbon nanotubes with ammonia increased the activity of Pd nanoparticles by forming surface amine groups.
DIAMOND AND RELATED MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Sajjad Ali, Rashid Iqbal, Azim Khan, Shafiq Ur Rehman, Muhammad Haneef, Lichang Yin
Summary: Support materials play a crucial role in determining the dispersion, utilization, and stability of single metal atoms as part of single-atom catalysts. Defective and doped graphene was explored as a potential support for CO2 conversion to formic acid by having higher adsorption energy for Cu, Pd, and Ru supported on it. Path B, involving H2 adsorption on the support material, was found to dominate the CO2 hydrogenation reaction with lower energy barriers, especially in the case of Pd supported on defective graphene.
ACS APPLIED NANO MATERIALS
(2021)
Article
Chemistry, Physical
Abdul Qadeer, Meiqi Yang, Yuejie Liu, Qinghai Cai, Jingxiang Zhao
Summary: In this study, the catalytic performance of single-atom catalysts (SACs) supported on graphitic carbon nitrides (g-CN) for the formic acid oxidation reaction (FAOR) was explored using density functional theory computations. The results showed that efficient FAOR can be achieved on Ru/g-CN catalysts through a direct pathway of HCOOH(aq) -> HCOOH* -> HCOO* -> CO2* -> CO2(g). This research provides a new approach to develop novel catalysts for sustainable FAOR in formic-acid-based fuel cells.
Article
Nanoscience & Nanotechnology
Xiang Li, Xinyuan Peng, Yixuan Wang, Bo Xi, Jingjing Dou, Jun-Jun Zhang, Yaming Liu, Changqing Jin
Summary: This study reports a method of enhancing the catalytic efficiency of Pd atoms by doping with Fe/Co atoms. The optimized compositions of PdFe and PdCo nanoparticles can be synthesized by controlling the doping amount of Fe/Co atoms. These nanoparticles exhibit significantly improved catalytic activity in the formic acid oxidation reaction.
ACS APPLIED NANO MATERIALS
(2022)
Review
Chemistry, Inorganic & Nuclear
Yuxi Zeng, Eydhah Almatrafi, Wu Xia, Biao Song, Weiping Xiong, Min Cheng, Ziwei Wang, Yuntao Liang, Guangming Zeng, Chengyun Zhou
Summary: Single-atom catalysts (SACs) combining the advantages of both heterogeneous and homogeneous catalysts have become the forefront in advanced oxidation processes (AOPs). Carbon-based single-atom Fe catalysts (Fe-SACs) with nitrogen doping have attracted attention in environmental catalysis due to their high activity, selectivity, and stability. However, there is a lack of comprehensive reviews on the use of carbon-based Fe-SACs for AOPs degradation of organic water pollution.
COORDINATION CHEMISTRY REVIEWS
(2023)
Article
Chemistry, Physical
Die Guo, Zhi Huang, Yanying Liu, Qian Zhang, Yanling Yang, Junming Hong
Summary: Combining metal and graphene catalysts as anode can improve the efficiency of electrocatalysis in degrading pharmaceutical contaminants such as acetaminophen. This research successfully fabricates single-atom copper and nitrogen codoped graphene as an electrocatalytic anode, achieving maximum utilization efficiency of copper atoms and optimizing the activity and stability of the catalyst.
APPLIED SURFACE SCIENCE
(2022)
Review
Materials Science, Multidisciplinary
Xianyang Zhang, Pengfei Chen, Siwuxie He, Bowen Jiang, Yong Wang, Yonghua Cheng, Jian Peng, Francis Verpoort, John Wang, Zongkui Kou
Summary: Biosensors featuring single molecule detection offer great opportunities in various fields, but face challenges due to the lack of activity, precision molecule selectivity, and understanding of the operating mechanism. Single-atom catalysts (SACs), particularly those that mimic the natural metalloenzyme structure, provide practical-use feasibilities for single molecule detections with high molecular selectivity and easy fabrication. This review discusses the history, advantages, and applications of SACs in molecule-scale biosensors, emphasizing their sensing modes and coordination-modulated signal amplifications.
Article
Chemistry, Multidisciplinary
Hu Liu, Qian Lei, Ruoyan Miao, Mingzi Sun, Chuanjian Qin, Liang Zhang, Gan Ye, Yao Yao, Bolong Huang, Zhenhui Ma
Summary: This study presents an asymmetrically coordinated metal single-atom catalyst for efficient dehydrogenation of formic acid. The catalyst exhibits impressive activity and stability, outperforming symmetrically coordinated catalysts and commercial catalysts.
ADVANCED FUNCTIONAL MATERIALS
(2022)