摘要
Photocatalytic hydrogen production represents a promising strategy for clean, sustainable, and environmentfriendly energy supply. Up to now, great efforts have been devoted to designing the photocatalysts with noble metal as co-catalyst for visible-light-driven hydrogen evolution, while more efficient photocatalytic systems are still a major challenge. Herein, we report a facile strategy for synthesizing faceto-face ultrathin Pd nanosheets-amorphous carbon nitride(Pd NSs-ACN) structure with large contacting interface and short electronic transmission pathway, which can work as an efficient photocatalyst for hydrogen production. The synthesis starts with the growth of ultrathin Pd NSs, followed by assembly with the visible-light-response ACN through a simple stirring and annealing procedure. The resultant two dimensional face-to-face structures deliver an average hydrogen generation rate of 1.45 mmol h-1g-1 at a temperature of 25℃,almost 2.6 times higher than that of Pd Nps-ACN with particle-to-face structural feature. The efficient photocatalytic activity is ascribed to the formation of high-density of active sites between ultrafine face-to-face contacted Pd NSs and the ACN, which cooperate more synergistically towards photocatalytic hydrogen production. The face-to-face engineered Pd NSs-ACN hybrids also offer a good stability revealed by photocatalytic hydrogen production measurements. The extraordinary performance highlights a powerful engineering model for designing other face-to-face contacting co-catalyst/photocatalysts, which will be a great impetus to optimize new catalytic transformations.
目前,能源与环境问题已经成为影响人类可持续发展的主要矛盾.为了实现人类社会的可持续发展,研究者们一直致力于开发新的储能技术.半导体光催化制氢凭借其清洁、可持续、环境友好的优势成为研究热点.传统的光催化制氢体系以贵金属为助催化剂,宽带隙半导体为光催化剂,这种光催化系统的太阳能转换效率难以满足实际需求.在本文中,我们合成出一种具有较大接触界面和较短的电子传递路径的共面型超薄钯纳米片/非晶氮化碳复合结构.在室温25℃条件下,该结构平均氢气生成速率为1.45 mmol mg^(-1)h^(-1),是钯纳米颗粒-无定形碳化氮粒面型结构的2.6倍.同时,该共面型光催化剂具有优良的产氢稳定性.该催化剂既充分利用了钯纳米片表面高密度的活性位点,又利用了无定型氮化碳宽的光谱响应.本工作为可见光驱动的高效助催化剂和光催化剂界面设计提供了一种新的策略.
基金
financially supported by the National Natural Science Foundation of China (51772255)
Hunan Natural Science Foundation (2016JJ3123)
the National Key Research and Development Program of China (2016YFB0100201)
the start-up supports from Peking University
Young Thousand Talented Program
