Chen Biao, Wang Dashuai, Zhang Biao, Zhong Xiongwei, Liu Yingqi, Sheng Jinzhi, Zhang Qi, Zou Xiaolong, Zhou Guangmin, Cheng Hui-Ming
Shenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, People's Republic of China.
School of Materials Science and Engineering and Tianjin Key Laboratory of Composite and Functional Materials, Tianjin University, Tianjin, 300350, People's Republic of China.
ACS Nano. 2021 Jun 22;15(6):9841-9850. doi: 10.1021/acsnano.1c00756. Epub 2021 May 25.
As one of the CO capture and utilization technologies, Li-CO 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 LiCO formation and decomposition remains challenging. Here, guided by theoretical calculations, CO was utilized to activate the catalytic activity of conventional nitrogen-doped graphene, in which pyridinic-N and pyrrolic-N have a high total content (72.65%) and have a high catalytic activity in both CO reduction and evolution reactions, thus activating the reversible conversion of LiCO formation and decomposition. As a result, the designed cathode has a low voltage gap of 2.13 V at 1200 mA g and long-life cycling stability with a small increase in the voltage gap of 0.12 V after 170 cycles at 500 mA g. Our work suggests a way to design metal-free catalysts with high activity that can be used to activate the performance of Li-CO batteries.
作为二氧化碳捕获与利用技术之一，锂-二氧化碳电池在碳中和应用中引起了特别关注。然而，设计和制造用于可逆碳酸锂形成与分解的低成本高效阴极催化剂仍然具有挑战性。在此，在理论计算的指导下，利用一氧化碳激活传统氮掺杂石墨烯的催化活性，其中吡啶氮和吡咯氮的总含量较高（72.65%），并且在一氧化碳还原和析出反应中均具有较高的催化活性，从而激活碳酸锂形成与分解的可逆转化。结果，所设计的阴极在1200 mA g时具有2.13 V的低电压间隙，并且具有长寿命循环稳定性，在500 mA g下循环170次后电压间隙仅小幅增加0.12 V。我们的工作提出了一种设计具有高活性的无金属催化剂的方法，可用于激活锂-二氧化碳电池的性能。
