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One-Dimensional Multichannel g-C3N4.7 Nanostructure Realizing an Efficient Photocatalytic Hydrogen Evolution Reaction and Its Theoretical Investigations
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2021-03-18 , DOI: 10.1021/acsaem.0c02858
Bindu Antil 1 , Lakshya Kumar 1 , Ravi Ranjan 2 , Sulakshana Shenoy 3 , Kartick Tarafder 3 , Chinnakonda S. Gopinath 2 , Sasanka Deka 1
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2021-03-18 , DOI: 10.1021/acsaem.0c02858
Bindu Antil 1 , Lakshya Kumar 1 , Ravi Ranjan 2 , Sulakshana Shenoy 3 , Kartick Tarafder 3 , Chinnakonda S. Gopinath 2 , Sasanka Deka 1
Affiliation
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The emerging metal-free carbon nitride (C3N4) offers prominent possibilities for realizing the highly effective hydrogen evolution reaction (HER). However, its poor surface conductivity and insufficient catalytic sites hinder the HER performance. Herein, a one-dimensional vermicular rope-like graphitic carbon nitride nanostructure is demonstrated that consists of multichannel tubular pores and high nitrogen content, which is fabricated through a cost-effective approach having the final stoichiometry g-C3N4.7 for HER application. The present g-C3N4.7 is unique owing to the presence of abundant channels for the diffusion process, modulated surface chemistry with rich-electroactive sites from N-electron lone pairs, greatly reduced recombination rate of photoexcited exciton pairs, and a high donor concentration (4.26 × 1017 cm3). The catalyst offers a visible-light-driven photocatalytic H2 evolution rate as high as 4910 μ mol h–1 g–1 with an apparent quantum yield of 14.07% at band gap absorption (2.59 eV, 479 nm) under 7.68 mW cm–2 illumination. The number of hydrogen gas molecules produced is 1.307 × 1015 s–1 cm–2, which remained constant for a minimum of 18 h of repeated cycling in the HER without any degradation of the catalyst. In density functional theory calculations, a significant change in the band offset is observed due to N doping into the system in favor of electron catalysis. The theoretical band gap of a monolayer of g-C3N4.7 was enormously reduced because of the presence of additional densities of states from the doped N atom inside the band gap. These impurity or donor bands are formed inside the band gap region, which ultimately enhance the hydrogen ion reduction reaction enormously.
中文翻译：
一维多通道gC 3 N 4.7纳米结构实现有效的光催化氢释放反应及其理论研究
新兴的不含金属的氮化碳（C 3 N 4）为实现高效的析氢反应（HER）提供了显着的可能性。然而，其差的表面电导率和不足的催化位点阻碍了HER性能。本文中，展示了一种由多通道管状孔和高氮含量组成的一维蠕状绳状石墨碳氮化物纳米结构，该结构是通过具有成本效益的方法制造的，该方法具有用于HER的最终化学计量比gC 3 N 4.7。目前的gC 3 N 4.7由于扩散过程中存在丰富的通道，具有来自N电子孤对的丰富电活性位点的调制表面化学，光激发激子对的重组率大大降低以及高施主浓度（4.26×10 17 cm 3）。催化剂提供的可见光驱动光催化ħ 2进化率高达4910μ摩尔ħ -1克-1与表观量子的14.07％在带隙吸收下7.68毫瓦厘米收率（2.59电子伏特，479纳米）- 2照明。产生的氢气分子数量为1.307×10 15 s –1 cm –2，在HER中至少18个小时的重复循环中保持恒定，且催化剂没有任何降解。在密度泛函理论计算中，由于N掺杂到系统中有利于电子催化，观察到了带隙的显着变化。gC 3 N 4.7单层的理论带隙被大大降低，因为在带隙内存在来自掺杂N原子的附加态密度。这些杂质或给体带形成在带隙区域内，最终极大地增强了氢离子还原反应。
更新日期：2021-04-26
中文翻译：
一维多通道gC 3 N 4.7纳米结构实现有效的光催化氢释放反应及其理论研究
新兴的不含金属的氮化碳（C 3 N 4）为实现高效的析氢反应（HER）提供了显着的可能性。然而，其差的表面电导率和不足的催化位点阻碍了HER性能。本文中，展示了一种由多通道管状孔和高氮含量组成的一维蠕状绳状石墨碳氮化物纳米结构，该结构是通过具有成本效益的方法制造的，该方法具有用于HER的最终化学计量比gC 3 N 4.7。目前的gC 3 N 4.7由于扩散过程中存在丰富的通道，具有来自N电子孤对的丰富电活性位点的调制表面化学，光激发激子对的重组率大大降低以及高施主浓度（4.26×10 17 cm 3）。催化剂提供的可见光驱动光催化ħ 2进化率高达4910μ摩尔ħ -1克-1与表观量子的14.07％在带隙吸收下7.68毫瓦厘米收率（2.59电子伏特，479纳米）- 2照明。产生的氢气分子数量为1.307×10 15 s –1 cm –2，在HER中至少18个小时的重复循环中保持恒定，且催化剂没有任何降解。在密度泛函理论计算中，由于N掺杂到系统中有利于电子催化，观察到了带隙的显着变化。gC 3 N 4.7单层的理论带隙被大大降低，因为在带隙内存在来自掺杂N原子的附加态密度。这些杂质或给体带形成在带隙区域内，最终极大地增强了氢离子还原反应。
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