Zhang W X, Yin Y, He C
School of Materials Science and Engineering, Chang'an University, Xi'an 710064, China.
State Key Laboratory for Mechanical Behavior of Materials, School of Materials Science and Engineering, Xi'an Jiaotong University, Xi'an 710049, China.
J Phys Chem Lett. 2021 Jun 3;12(21):5064-5075. doi: 10.1021/acs.jpclett.1c01023. Epub 2021 May 24.
With the aggravation of environmental pollution and the energy crisis, it is particularly important to develop and design environment-friendly and efficient spontaneous enhanced visible-light-driven photocatalysts for water splitting. Herein novel type-II van der Waals (vdW) GaSe/CN and GaSSe/CN heterostructures are proposed through first-principles calculations. Their electronic properties and photocatalytic performance are theoretically analyzed. In particular, their appropriate band gap and band-edge position meet the requirements of the oxygen evolution reaction, and the reaction is thermodynamically feasible in most pH ranges. The unique band alignment of these heterostructured photocatalysts leads to high solar-to-hydrogen energy conversion efficiencies up to 15.11%, which has a good commercial application prospect. More excitingly, with the application of 2% biaxial strain, the smooth progress of the water-splitting reaction of the GaSe/CN and GaSSe/CN heterostructures can still be maintained, and the carrier mobility and optical absorption characteristics can be effectively improved. Consequently, these findings suggest that the GaSe/CN and GaSSe/CN vdW heterostructures have promising potentials as photocatalysts for water splitting. This work may provide a promising clue for the design of efficient and stable photocatalytic water-splitting catalysts under visible spectroscopy.
随着环境污染和能源危机的加剧，开发和设计环境友好且高效的自发增强可见光驱动的光催化剂用于水分解变得尤为重要。在此，通过第一性原理计算提出了新型II型范德华（vdW）GaSe/CN和GaSSe/CN异质结构。对它们的电子性质和光催化性能进行了理论分析。特别地，它们合适的带隙和带边位置满足析氧反应的要求，并且该反应在大多数pH范围内在热力学上是可行的。这些异质结构光催化剂独特的能带排列导致高达15.11%的高太阳能到氢能转换效率，具有良好的商业应用前景。更令人兴奋的是，施加2%的双轴应变时，GaSe/CN和GaSSe/CN异质结构的水分解反应仍能顺利进行，并且载流子迁移率和光吸收特性可以得到有效改善。因此，这些发现表明GaSe/CN和GaSSe/CN vdW异质结构作为水分解光催化剂具有广阔的潜力。这项工作可能为可见光谱下高效稳定的光催化水分解催化剂的设计提供一个有前景的线索。
