Carbon Nitride Co-Catalyst Activation Using N-doped Carbon with Enhanced Photocatalytic H2 Evolution.
Carbon Nitride Co-Catalyst Activation Using N-doped Carbon with Enhanced Photocatalytic H2 Evolution.
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DOI：
10.1021/acs.langmuir.9b01796
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发表时间：
2019-08
期刊：
影响因子：
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通讯作者：
Jianhai Wang;Qing Zhou;Yanfei Shen;Xinghua Chen;Songqin Liu;Yuanjian Zhang
中科院分区：
文献类型：
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作者：
Jianhai Wang;Qing Zhou;Yanfei Shen;Xinghua Chen;Songqin Liu;Yuanjian Zhang
光催化水分解在应对当前能源和环境挑战方面具有巨大的潜力。其中，聚合物氮化碳（CN）作为一种很有前途的无金属光催化剂而备受关注。众所周知，许多有前途的共催化剂已经被开发出来以改善催化反应，Pt纳米粒子仍然是CN光催化析氢的最佳共催化剂之一，因为它具有合适的费米能级来转移激发态电子和H2还原的低过电位。本文报道了采用少量n掺杂碳（N-C）作为过渡层的尿素衍生体CN和Pt共催化剂的界面工程，其光催化活性提高了7倍。结果表明，在N-C的存在下，水还原Pt共催化剂的活化能降低，CN与N-C的密切相互作用促进了载流子的有效分离和迁移，这是由于N-C的元素组成和晶体结构相似。本研究为利用光催化剂/助催化剂界面工程开发具有更高活性的cn基太阳能燃料转化光催化剂开辟了新的途径。
Photocatalytic water splitting holds huge potential to meet the current challenges of energy and environments. Among them, polymeric carbon nitride (CN) has drawn much attention as a promising metal-free photocatalyst. As known, a number of promising co-catalysts have been developed to improve catalytic reactions, Pt nanoparticles is still among the best co-catalysts for CN in photocatalytic H2 evolution, due to the its suitable Fermi level to transfer excited electrons and the low overpotential for H2 reduction. Herein, we report the interface engineering of urea-derived bulk CN and Pt co-catalyst by using a small portion of N-doped carbon (N-C) as transition layer with a boosted photocatalytic activity up to 7 times. It was revealed that the activation energy of Pt co-catalyst for water reduction was lowered in the presence of N-C, and the intimate interaction between CN and N-C, ascribing to the similar elemental composition and crystal structure, promoted the efficient separation and migration of charge carriers. This study may open a new avenue to develop CN-based photocatalysts for solar fuel conversion with even higher activity by photocatalyst/co-catalyst interface engineering.