摘要
A hexagonal boron carbon nitride(h-BCN) semiconductor was applied to intercalate cobalt ions to catalyze oxygen evolution reaction(OER) with light illumination, without using noble metals. The h-BCN with high specific surface area showed a strong chemical affinity towards metal ions due to the 'lop-sided' densities characteristic of ionic B–N bonding, enabling the creation of metal/h-BCN hybrid layered structures with unique properties. As exemplified here by Co/h-BCN for water oxidation catalysis, after intercalating cobalt ions in the h-BCN host, the photocatalytic activity of the resultant layered hybrid is optimized due to their synergic catalysis that promotes charge separation and lowers reaction barriers. This finding promises a new nobel-metal-free nanocompsite using cost-acceptable and earth-abundant sustances for photocatalytic OER, and enables the facile design of duel catalytic cascades by merging transition metal catalysis with h-BCN(photo)catalysis for energy and sustainability.
本文利用六方相硼氮碳(h-BCN)半导体光催化剂吸附钴离子,构筑不含任何贵金属成分的光催化体系,在可见光照射下,实现水的催化氧化生成氧气反应.h-BCN半导体材料由于B–N离子键的"lop-sided"效应,对金属离子具有很强的化学亲和性,利用此性质并结合其高比表面积的特性,制备出了一系列具有特殊性能的金属/h-BCN杂化层状结构.研究结果表明,在钴离子镶嵌的h-BCN(Co/h-BCN)杂化材料中,金属和载体之间的协同作用能有效促进光生载流子分离、降低反应活化能,进而提高光催化氧化水产氧性能.本文展示了利用廉价和地球高丰度元素构筑不含贵金属成份的纳米层状复合材料,有望将过渡金属催化和h-BCN光催化耦合,实现面向可持续能源转换的协同催化过程.
基金
supported by the National Basic Research Program of China (2013CB632405)
the National Natural Science Foundation of China (21425309 and 21173043)