Cheng Yongtai, Wu Haofei, Han Jiuhui, Zhong Siying, Huang Senhe, Chu Shufen, Song Shuangxi, Reddy Kolan Madhav, Wang Xiaodong, Wu Shaoyi, Zhuang Xiaodong, Johnson Isaac, Liu Pan, Chen Mingwei
Shanghai Key Laboratory of Advanced High-temperature Materials and Precision Forming, State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. China.
Frontier Research Institute for Interdisciplinary Sciences (FRIS), Tohoku University, Sendai 980-8577, Japan and WPI Advanced Institute for Materials Research, Tohoku University, Sendai 980-8577, Japan.
Nanoscale. 2021 Jun 24;13(24):10862-10870. doi: 10.1039/d1nr01612a.
Highly active, cost-effective and durable electrocatalysts for the oxygen reduction reaction (ORR) are critically important for renewable energy conversion and storage. Here we report a 3D bicontinuous nitrogen doped nanoporous graphene electrocatalyst co-anchoring with atomically dispersed nickel and copper atoms ((Ni,Cu)-NG) as a highly active single-atom ORR catalyst, fabricated by the combination of chemical vapor deposition and high temperature gas transportation. The resultant (Ni,Cu)-NG exhibits an exceptional ORR activity in alkaline electrolytes, comparable to the Pt-based benchmarks, from the synergistic effect of the CuNx and NiNx complexes. Endowed with high catalytic activity and outstanding durability under harsh electrochemical environments, rechargeable zinc-air batteries using (Ni,Cu)-NG as the cathodes show excellent energy efficiency (voltage gap of 0.74 V), large power density (150.6 mW cm-2 at 250 mA cm-2) and high cycling stability (>500 discharge-charge cycles at 10 mA cm-2). This study may pave an efficient avenue for designing highly durable single-atom ORR catalysts for metal-air batteries.
用于氧还原反应（ORR）的高活性、高性价比且耐用的电催化剂对于可再生能源的转换和存储至关重要。在此，我们报道了一种三维双连续氮掺杂纳米多孔石墨烯电催化剂，它与原子级分散的镍和铜原子共同锚定（(Ni,Cu)-NG），作为一种高活性单原子ORR催化剂，通过化学气相沉积和高温气体传输相结合的方法制备而成。所得的(Ni,Cu)-NG在碱性电解质中表现出卓越的ORR活性，与基于铂的基准催化剂相当，这得益于CuNx和NiNx络合物的协同效应。由于在苛刻的电化学环境下具有高催化活性和出色的耐久性，使用(Ni,Cu)-NG作为阴极的可充电锌空气电池表现出优异的能量效率（电压差为0.74 V）、高功率密度（在250 mA cm-2时为150.6 mW cm-2）和高循环稳定性（在10 mA cm-2下>500次充放电循环）。这项研究可能为设计用于金属空气电池的高度耐用的单原子ORR催化剂开辟一条有效途径。
