期刊
ACS NANO
卷 15, 期 6, 页码 9841-9850出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.1c00756
关键词
graphene; nitrogen configuration; active site; CO2 activation; Li-CO2 batteries
类别
资金
- China Postdoctoral Science Foundation [2020TQ0159, 2020M680544, 2020M680506]
- Guangdong Innovative and Entrepreneurial Research Team Program [2017ZT07C341]
- National Key Research and Development Program of China [2019YFA0705700]
- National Natural Science Foundation of China [52072205]
- Tsinghua Shenzhen International Graduate School
- Shenzhen Geim Graphene Center
- Bureau of Industry and Information Technology of Shenzhen [201901171523]
- Foundation of Science and Technology on Surface Physics and Chemistry Laboratory [WDZC201901]
This study utilized CO2 to activate the catalytic activity of nitrogen-doped graphene, enabling the design of a low-cost high-efficiency cathode catalyst for Li-CO2 batteries. The cathode exhibited a low voltage gap and long-life cycling stability, suggesting a way to design metal-free catalysts with high activity for improved Li-CO2 battery performance.
As one of the CO2 capture and utilization technologies, Li-CO2 batteries have attracted special interest in the application of carbon neutral. However, the design and fabrication of a low-cost high-efficiency cathode catalyst for reversible Li2CO3 formation and decomposition remains challenging. Here, guided by theoretical calculations, CO2 was utilized to activate the catalytic activity of conventional nitrogen-doped graphene, in which pyridinic-N and pyrrolic-N have a high total content (72.6590) and have a high catalytic activity in both CO2 reduction and evolution reactions, thus activating the reversible conversion of Li2CO3 formation and decomposition. As a result, the designed cathode has a low voltage gap of 2.13 V at 1200 mA g(-1) and long-life cycling stability with a small increase in the voltage gap of 0.12 V after 170 cycles at 500 mA g(-1). Our work suggests a way to design metal-free catalysts with high activity that can be used to activate the performance of Li-CO2 batteries.
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