Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-12-10 , DOI: 10.1016/j.apcatb.2020.119806 Jinzhu Ma , Yingfa Chen , Guangzhi He , Hong He
Numerous catalytic reaction systems take oxygen vacancy as the active site to initiate the redox cycle. However, the oxygen vacancy is easily occupied by various oxygen-containing species (e.g., water or other intermediates), resulting in catalyst deactivation. Here, we demonstrate that the layered double hydroxide (LDH) catalysts fundamentally solve the deactivation of oxygen vacancy frequently encountered with metal oxide catalyst systems, which simultaneously realizes the superior reactivity and durability for catalyzing ozone decomposition. First-principles calculations reveal that the ubiquitous surface hydroxyls on the layered hydroxide serve as the reactive sites and the redox cycle is achieved by a robust H-transfer mechanism in the 2D confined LDH systems, which are responsible for the extraordinary activity and resistance of LDH catalysts.
中文翻译:
强大的H转移氧化还原机制决定了层状双氢氧化物的高效催化性能
许多催化反应系统将氧空位作为活性部位来引发氧化还原循环。然而,氧空位容易被各种含氧物质(例如水或其他中间体)所占据,导致催化剂失活。在这里,我们证明了层状双氢氧化物(LDH)催化剂从根本上解决了金属氧化物催化剂体系经常遇到的氧空位失活问题,同时实现了出色的反应性和耐久性,可催化臭氧分解。第一性原理计算表明,层状氢氧化物上无处不在的表面羟基充当反应位点,氧化还原循环是通过二维受限LDH系统中强大的H转移机制实现的,