Gang Dong*, Tianxiang Zhou, Chengzhi Zhang, Yongchao Wang, Yang Wang*, Wei Shi, Xiaoli Su, Tao Zeng and Yunxia Chen*,
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引用次数: 0
Abstract
Constructing a heterojunction is an effective way to overcome the handicaps of single-component photocatalysts for the photocatalytic N2 reduction reaction (PNRR). However, the fundamental photophysical processes between two semiconductors with different nanostructures are still unclear. Drawing upon a combination of experimental observations and theoretical calculations, a series of binary nanohybrid photocatalysts of MoS2 (nanodot, monolayer, and few nanolayers) and carbon nitride are systematically evaluated as potential N2 reduction reaction photocatalysts. Owing to the atomically well-defined interfacial interaction between MoS2 and graphitic carbon nitride (GCN), charge accumulates in MoS2. Meanwhile, the electron density of MoS2 increases with the reduction of nanosize, thereby facilitating N2 adsorption on the Mo-edge and boosting the potential-determining step of the desorption of the NH3 molecule. Simultaneously, the MoS2 nanodot anchored on GCN manifests a compelling photothermal effect upon solar light irradiation and raises the temperature of the compound in situ, leading to efficient charge transfer and thereby enhancing the photocatalytic performance. Encouragingly, the final product reaches a high ammonia synthesis rate of 2.71 mmol h–1 g–1 at ambient conditions and an apparent quantum of 0.62% at 430 nm. Establishing the relationship between the nano-, electronic structure and PNRR performance of MoS2/GCN heterojunction materials provides valuable insights for their potential application in PNRR technology.
期刊介绍:
ACS Applied Nano Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics and biology relevant to applications of nanomaterials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important applications of nanomaterials.