He Guanjie, Qiao Mo, Li Wenyao, Lu Yao, Zhao Tingting, Zou Rujia, Li Bo, Darr Jawwad A, Hu Junqing, Titirici Maria-Magdalena, Parkin Ivan P
Christopher Ingold Laboratory Department of Chemistry University College London 20 Gordon Street London WC1H 0AJ UK.
School of Engineering and Materials Science/Materials Research Institute Queen Mary University of London Mile End Road E14NS London UK.
Adv Sci (Weinh). 2016 Aug 17;4(1):1600214. doi: 10.1002/advs.201600214. eCollection 2017 Jan.
Metal sulfides are commonly used in energy storage and electrocatalysts due to their redox centers and active sites. Most literature reports show that their performance decreases significantly caused by oxidation in alkaline electrolyte during electrochemical testing. Herein, S and N co-doped graphene-based nickel cobalt sulfide aerogels are synthesized for use as rechargeable alkaline battery electrodes and oxygen reduction reaction (ORR) catalysts. Notably, this system shows improved cyclability due to the stabilization effect of the S and N co-doped graphene aerogel (SNGA). This reduces the rate of oxidation and the decay of electronic conductivity of the metal sulfides materials in alkaline electrolyte, i.e., the capacity decrease of CoNiS/SNGA is 4.2% for 10 000 cycles in a three-electrode test; the current retention of 88.6% for Co-S/SNGA after 12 000 s current-time chronoamperometric response in the ORR test is higher than corresponding Co-S nanoparticles and Co-S/non-doped graphene aerogels. Importantly, the results here confirm that the Ni-Co-S ternary materials behave as an electrode for rechargeable alkaline batteries rather than supercapacitors electrodes in three-electrode test as commonly described and accepted in the literature. Furthermore, formulas to evaluate the performance of hybrid battery devices are specified.
金属硫化物因其氧化还原中心和活性位点而常用于能量存储和电催化剂。大多数文献报道表明,在电化学测试过程中,它们在碱性电解质中的氧化会导致其性能显著下降。在此,合成了硫和氮共掺杂的石墨烯基镍钴硫化物气凝胶,用作可充电碱性电池电极和氧还原反应(ORR)催化剂。值得注意的是,由于硫和氮共掺杂的石墨烯气凝胶(SNGA)的稳定作用,该体系显示出改善的循环稳定性。这降低了金属硫化物材料在碱性电解质中的氧化速率和电子电导率的衰减,即在三电极测试中,CoNiS/SNGA在10000次循环后的容量下降为4.2%;在ORR测试中,Co-S/SNGA在12000秒电流-时间计时电流响应后的电流保留率为88.6%,高于相应的Co-S纳米颗粒和Co-S/未掺杂石墨烯气凝胶。重要的是,这里的结果证实,在三电极测试中,Ni-Co-S三元材料表现为可充电碱性电池的电极,而不是如文献中通常描述和接受的超级电容器电极。此外,还给出了评估混合电池装置性能的公式。