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通过空间电荷分离合理设计的TiC/N,S-TiO/g-CN三元异质结构用于增强光催化析氢

Rationally designed TiC/N, S-TiO/g-CN ternary heterostructure with spatial charge separation for enhanced photocatalytic hydrogen evolution.

作者信息

Biswal Lijarani, Nayak Susanginee, Parida Kulamani

机构信息

Centre for Nano Science and Nano Technology, Institute of Technical Education and Research, Siksha 'O' Anusandhan Deemed to be University, Bhubaneswar 751030, Odisha, India.

Centre for Nano Science and Nano Technology, Institute of Technical Education and Research, Siksha 'O' Anusandhan Deemed to be University, Bhubaneswar 751030, Odisha, India.

出版信息

J Colloid Interface Sci. 2022 Sep;621:254-266. doi: 10.1016/j.jcis.2022.04.071. Epub 2022 Apr 15.

Abstract

The charge separation and transfer are the major issues dominating the under-laying energy conversion mechanism for photocatalytic system. Construction of semiconductor-based heterojunction system considered to be viable option for boosting the spatial charge separation and transfer in the photocatalytic water splitting system. Here, we design a ternary heterojunction of TiC/N, S-TiO/g-CN by thermal annealing and ultrasonic assisted impregnation method having a well-designed n-n heterojunction and noble metal free Schottky junction for adequate hydrogen evolution. The optimal content of 4 wt% TiC on N, S-TiO/g-CN (4-TC/NST/CN) exhibit the highest rate of hydrogen generation 495.06μ mol h which is 3.1, 4.1 and 1.6 fold higher than the pristine N, S doped-TiO, g-CN and binary hybrid (N, S doped-TiO/g-CN) respectively, with 7% apparent conversion efficiency (ACE). The increment in the activity is described to the robust photogenerated carrier separation and double charge transfer channels because of the formation of dual heterojunction (n-n heterojunction and Schottky junction). XRD and Raman results revealed the occupancy of TiC in the heterojunction due to the strong interaction between TiC with N, S doped-TiO and g-CN. The HRTEM analysis confirmed the formation of close interfacial junction between the TiC, N, S doped-TiO and g-CN. Moreover, the higher photocurrent, low PL intensity and lower impedance arc suggested the lower charge carrier recombination rate in 4-TC/NST/CN heterojunction. This work represents a significant development to establish a sound foundation for future design of MXene-based ternary hybrid system towards significant charge carrier separation and transfer for H production activity.

摘要

电荷分离和转移是主导光催化系统底层能量转换机制的主要问题。构建基于半导体的异质结系统被认为是促进光催化水分解系统中空间电荷分离和转移的可行选择。在此,我们通过热退火和超声辅助浸渍法设计了TiC/N,S-TiO₂/g-C₃N₄三元异质结,其具有精心设计的n-n异质结和无贵金属肖特基结,以实现充足的析氢。N,S-TiO₂/g-C₃N₄上4 wt% TiC(4-TC/NST/CN)的最佳含量表现出最高的产氢速率为495.06 μmol h⁻¹,分别比原始的N,S掺杂TiO₂、g-C₃N₄和二元杂化物(N,S掺杂TiO₂/g-C₃N₄)高3.1倍、4.1倍和1.6倍,表观转换效率(ACE)为7%。活性的增加归因于由于双异质结(n-n异质结和肖特基结)的形成而实现的强大光生载流子分离和双电荷转移通道。XRD和拉曼结果表明,由于TiC与N,S掺杂TiO₂和g-C₃N₄之间的强相互作用,TiC存在于异质结中。HRTEM分析证实了TiC、N,S掺杂TiO₂和g-C₃N₄之间形成了紧密的界面结。此外,更高的光电流、更低的PL强度和更低的阻抗弧表明4-TC/NST/CN异质结中的电荷载流子复合率更低。这项工作代表了一项重大进展,为未来基于MXene的三元混合系统设计奠定了坚实基础,以实现用于产氢活性的显著电荷载流子分离和转移。

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