关键词: 0D/2D heterojunction Ag(2)S QDs Graphdiyne Infrared excited hydrogen production Photocatalytic hydrogen evolution

来  源:   DOI:10.1016/j.jcis.2024.06.065

Abstract:
Precisely crafting heterojunctions for efficient charge separation is a major obstacle in the realm of photocatalytic hydrogen evolution. A 0D/2D heterojunction was successfully fabricated by anchoring Ag2S quantum dots (Ag2S QDs) onto graphdiyne (GDY) nanosheets (Ag2S QDs/GDY) using a straightforward physical mixing technique. This unique structure allows for excellent contact between GDY and Ag2S QDs, thereby enhancing the rate of charge transfer. The light absorption capabilities of Ag2S QDs/GDY extend up to 1200 nm, enabling strong absorption of light, including infrared. Through DFT calculations and in-situ XPS analysis, it was demonstrated that incorporating Ag2S QDs onto GDY effectively modulates the electronic structure, promotes an internal electric field, and facilitates directional electron transfer. This directed electron transfer enhances the utilization of electrons by GDY and Ag2S QDs, with the added benefit of Ag2S QDs serving as electron reservoirs for efficient photocatalytic hydrogen evolution. A 7 %Ag2S QDs/GDY composite exhibited impressive efficiency and stable performance in photocatalytic hydrogen evolution (2418 μmol g-1 h-1), which is much higher than that of GDY and Ag2S QDs. This study conclusively demonstrates that the 0D/2D heterojunction formed by GDY and Ag2S QDs can establish high-quality contact and efficient charge transfer, ultimately enhancing photocatalytic performance.
摘要:
精确制作异质结以实现有效的电荷分离是光催化析氢领域的主要障碍。通过使用简单的物理混合技术将Ag2S量子点(Ag2SQD)锚定到石墨炔(GDY)纳米片(Ag2SQD/GDY)上,成功地制造了0D/2D异质结。这种独特的结构允许GDY和Ag2SQD之间的良好接触,从而提高电荷转移的速率。Ag2SQDs/GDY的光吸收能力高达1200nm,能够强烈吸收光,包括红外线。通过DFT计算和原位XPS分析,证明了将Ag2S量子点结合到GDY上可以有效地调节电子结构,促进内部电场,并促进定向电子转移。这种定向电子转移增强了GDY和Ag2SQD对电子的利用,与Ag2S量子点作为电子储库的有效光催化析氢的额外好处。7%的Ag2SQDs/GDY复合材料在光催化析氢(2418μmolg-1h-1)中表现出令人印象深刻的效率和稳定性能,远高于GDY和Ag2SQD。这项研究最终证明了GDY和Ag2S量子点形成的0D/2D异质结可以建立高质量的接触和高效的电荷转移,最终提高光催化性能。
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