Phosphorous doped graphitic-C3N4 hierarchical architecture for hydrogen production from water under visible light
Phosphorous doped graphitic-C3N4 hierarchical architecture for hydrogen production from water under visible light
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DOI：
10.1016/j.mtener.2017.05.006
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发表时间：
2017-09
影响因子：
9.3
通讯作者：
Linfei Zhang;Yi Zhang;R. Shi;Shuhan Bao;Jingwei Wang;Abbas Amini;B. Chandrashekar;Chun Cheng
中科院分区：
文献类型：
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作者：
Linfei Zhang;Yi Zhang;R. Shi;Shuhan Bao;Jingwei Wang;Abbas Amini;B. Chandrashekar;Chun Cheng
通过回流处理的乙烯二磷酸-三聚氰胺复合纤维网络直接煅烧制备富集大孔/介孔石墨-C3 N4（g-C3 N4）微棒（CNR）。优化的磷掺杂CNRs（P-CNRs）具有4960 μmol h−1g−1的高析氢速率（是原始g-C3 N4的5.5倍）和显著的循环稳定性。P-CNRs的结构和电子性质的改变是其性能显著提高的主要原因。CNR的这种独特的分级结构增强了光散射，并提供了高的比表面积，从而提供了更多的催化活性位点。P掺杂大大增加了g-C3 N4的可见光吸收，使禁带宽度变窄。它还导致在导带的密度状态的提升，如所揭示的电子顺磁共振（EPR）谱。从P-CNRs的光致发光和光电流测量中观察到的强可见光发射猝灭意味着增强的电荷转移/分离过程。这项工作提出了一个非常简单和直接的方法，设计和开发高性能的可见光驱动的制氢催化剂。
Enriched macro/mesoporous graphitic-C3N4(g-C3N4) micro-rods (CNRs) are prepared by direct calcination of reflux treated ethylene diphosphonic acid-melamine complex fiber network. The optimized phosphorous doped CNRs (P-CNRs) exhibit a high hydrogen-evolution rate of 4960 μmol h−1g−1(5.5 times that of pristine g-C3N4) with a remarkable recycling stability. The significantly enhanced performance is found to be attributed to the intentionally designed morphology and electronic properties of P-CNRs. This distinctive hierarchical architecture of CNRs enhances the light scattering, and provides a high specific surface area and thus more catalytically active sites. The P doping of g-C3N4greatly increases the visible light absorption, narrows the band gap. It also results in a boost in the density state of the conduction band as revealed by the electron paramagnetic resonance (EPR) spectra. The strong visible light emission quenching, observed from the photoluminescence of P-CNRs and photocurrent measurements, implies an enhanced charge transfer/separation process. This work presents a very simple and direct method of designing and developing high-performance visible light driven catalysts for hydrogen production.