Effects of composition faults in ternary metal chalcogenides (Zn In2S3+, x = 1–5) layered crystals for visible-light-driven catalytic hydrogen generation and carbon dioxide reduction
Effects of composition faults in ternary metal chalcogenides (Zn In2S3+, x = 1–5) layered crystals for visible-light-driven catalytic hydrogen generation and carbon dioxide reduction
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DOI：
10.1016/j.apcatb.2019.117810
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发表时间：
2019-11
期刊：
影响因子：
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通讯作者：
Yan Wu;Hou Wang;Wenguang Tu;Shuyang Wu;J. Chew
中科院分区：
文献类型：
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作者：
Yan Wu;Hou Wang;Wenguang Tu;Shuyang Wu;J. Chew
开发高效、稳定的光催化剂是光催化分解水制备清洁氢燃料的关键。本工作通过简单的水热法合成了具有不同组分缺陷的ZnxIn 2S 3 +x（x= 1-5）系列高效可见光催化剂。ZnxIn 2S 3 + x样品中的组分缺陷在载流子从内表面到外表面的转移中起着重要作用，进一步影响了光生电子和空穴在固液界面的氧化还原反应。ZnxIn 2S 3 + x样品的吸收边随着合成溶液中Zn/In原子比的增加而向较短波长移动（即，x从1增加到5）。通过可见光下光催化水制氢和CO2还原反应评价了ZnxIn 2S 3 + x的光催化活性。在ZnxIn 2S 3 + x光催化剂中，ZnIn 2S 4（x= 1）样品表现出最好的光催化活性，其析氢速率为2.93 mmol·h-1g-1，420 nm处的量子产率为7.92%。至于可见光驱动的CO2还原，ZnIn 2S 4样品也表现出最高的CO生成速率，为40.4 μmol h−1g−1。结果表明，成分缺陷的存在提供了额外的能量障碍，阻止光生载流子转移。此外，循环测试表明ZnIn 2S 4产品在重复使用的五个循环中具有稳定性。该研究为揭示ZnxIn 2S 3 + x层状晶体的结构-性能关系提供了新的见解，这对于在广泛的环境能源应用中的实施具有价值。
Exploring efficient and stable photocatalysts is critical for the practical application of photocatalytic water splitting to get clean hydrogen fuel. In this work, ZnxIn2S3+x(x= 1–5) samples with various composition faults were synthesized through a simple hydrothermal method as a series of highly efficient visible-light-driven photocatalysts. Composition faults in ZnxIn2S3+xsamples played important roles in the charge carrier transfer from internal to external surfaces, further affecting the redox reaction of photogenerated electrons and holes at the solid-liquid interface. The absorption edge of ZnxIn2S3+xsamples shifted to shorter wavelengths as the atomic ratio of Zn/In in the synthetic solution was increased (i.e.,xincreased from 1 to 5). The photocatalytic activity of ZnxIn2S3+xwas evaluated via photocatalytic hydrogen production from water and CO2reduction under visible light irradiation. The obtained ZnIn2S4(x= 1) sample displayed the best photocatalytic activity among the ZnxIn2S3+xphotocatalysts, with the hydrogen evolution rate determined to be 2.93 mmol·h−1g−1and the quantum yield at 420 nm determined to be 7.92%. As for visible light-driven CO2reduction, the ZnIn2S4sample also exhibited the highest CO formation rate of 40.4 μmol h−1g−1. Results suggest that the existence of composition faults provided extra energy barriers to block photoinduced charge carrier transfer. Furthermore, the cyclic tests indicate the stability of the ZnIn2S4product over five cycles of repeated use. This study provides new insights into unveiling the relationship of structure-property of ZnxIn2S3+xlayered crystals, which are valuable for implementation in a wide range of environmental energy applications.