摘要
Development of efficient molecular devices for overall water splitting has always been a hotspot of research to realize clean and sustainable energy conversion. In the case, long-term durability of molecular devices is a crucial factor to determine their practical application. Here, an efficient composite molecular anode was assembled by immobilization of charge-neutral mononuclear Ru1 complex on COOHfunctionalized multiwalled carbon nanotubes(MWCNTs COOH) sticking on a glassy carbon(GC) electrode(Ru1/MWCNTsCOOH/GC). The prepared hybrid anode showed a low onset overpotential of only 380 mV for electrocatalytic water oxidation. Moreover, the anode displayed a steady catalytic current density of1.25 mA/cm^2 for more than 5 h at the overpotential of 580 m V, a high TON of 186000(5 h), a TOF of10.3 s-1 and a faradic efficiency of 96%, indicating the significant efficiency and extremely durability.The excellent durability of the molecular anode should be attributed to the key charge-neutral catalytic intermediates(Ru1 ad) of the catalytic step and the two long flexible carbon chains of the catalyst.
Development of efficient molecular devices for overall water splitting has always been a hotspot of research to realize clean and sustainable energy conversion. In the case, long-term durability of molecular devices is a crucial factor to determine their practical application. Here, an efficient composite molecular anode was assembled by immobilization of charge-neutral mononuclear Ru1 complex on COOHfunctionalized multiwalled carbon nanotubes（MWCNTs COOH） sticking on a glassy carbon（GC） electrode（Ru1/MWCNTsCOOH/GC）. The prepared hybrid anode showed a low onset overpotential of only 380 mV for electrocatalytic water oxidation. Moreover, the anode displayed a steady catalytic current density of1.25 mA/cm2 for more than 5 h at the overpotential of 580 m V, a high TON of 186000（5 h）, a TOF of10.3 s-1 and a faradic efficiency of 96%, indicating the significant efficiency and extremely durability.The excellent durability of the molecular anode should be attributed to the key charge-neutral catalytic intermediates（Ru1 ad） of the catalytic step and the two long flexible carbon chains of the catalyst.
基金
supported by the National Natural Science Foundation of China(21573033,21875030)
the National Basic Research Program of China(973 program,2014CB239402)
the Fundamental Research Funds for the Central Universities(DUT18ZD210)
the State Key Laboratory of Fine Chemicals(KF1610)
