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Graphitic Carbon Nitride/CdSe Quantum Dot/Iron Carbonyl Cluster Composite for Enhanced Photocatalytic Hydrogen Evolution
ACS Applied Nano Materials ( IF 5.9 ) Pub Date : 2021-06-09 , DOI: 10.1021/acsanm.1c01096 Chuanshuai Li 1 , Xianshao Zou 1 , Weihua Lin 1 , Hassan Mourad 1 , Jie Meng 2 , Yang Liu 1 , Mohamed Abdellah 1 , Meiyuan Guo 1 , Kaibo Zheng 1, 2 , Ebbe Nordlander 1
ACS Applied Nano Materials ( IF 5.9 ) Pub Date : 2021-06-09 , DOI: 10.1021/acsanm.1c01096 Chuanshuai Li 1 , Xianshao Zou 1 , Weihua Lin 1 , Hassan Mourad 1 , Jie Meng 2 , Yang Liu 1 , Mohamed Abdellah 1 , Meiyuan Guo 1 , Kaibo Zheng 1, 2 , Ebbe Nordlander 1
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A g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite has been successfully constructed. The structure and chemical composition of the composite were investigated via, inter alia, transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS). The ability of the assembly to act as a photocatalyst for proton reduction to form hydrogen gas was studied. With visible light irradiation for 4 h, the total H2 production catalyzed by the g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite was found to be 9 times as high as a corresponding CdSe/[Fe2S2(CO)6] assembly and significantly higher than either the CdSe quantum dots or g-C3N4 alone. The g-C3N4 support/matrix was found to enhance the stability and efficiency of the CdSe quantum dot/iron carbonyl cluster assembly in the photocatalytic hydrogen evolution process. Results from recycling tests showed that the g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite is a sustainable and robust photocatalyst, maintaining the same activity after three cycles. The photoinduced charge carrier transfer dynamics in the g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite system has been investigated by transient absorption (TA) and time-resolved photoluminescence (TRPL) spectroscopies. The spectroscopic results indicate efficient hole transfer from the valence band of the excited CdSe quantum dots to the molecular iron carbonyl clusters and from the defect state of the quantum dots to g-C3N4 in the g-C3N4/CdSe quantum dot/[Fe2S2(CO)6] composite, which significantly inhibits the recombination of photogenerated charge carriers in CdSe quantum dots and boosts the photocatalytic activity and stability for hydrogen evolution. Energy transfer from g-C3N4 to the CdSe quantum dot/[Fe2S2(CO)6] assembly with a time constant of 0.7 ns also contributed to the charge transfer process.
中文翻译：
用于增强光催化产氢的石墨氮化碳/CdSe量子点/羰基铁簇复合材料
成功构建了gC 3 N 4 /CdSe量子点/[Fe 2 S 2 (CO) 6 ]复合材料。复合材料的结构和化学成分尤其通过透射电子显微镜 (TEM)、傅里叶变换红外光谱 (FTIR) 和 X 射线光电子能谱 (XPS) 进行研究。研究了该组件作为质子还原形成氢气的光催化剂的能力。在可见光照射 4 小时后，gC 3 N 4 /CdSe 量子点/[Fe 2 S 2 (CO) 6催化的总 H 2生成] 复合材料被发现是相应的 CdSe/[Fe 2 S 2 (CO) 6 ] 组件的9 倍，并且显着高于单独的 CdSe 量子点或 gC 3 N 4。发现gC 3 N 4载体/基质在光催化析氢过程中提高了 CdSe 量子点/羰基铁簇组装的稳定性和效率。回收试验结果表明，gC 3 N 4 /CdSe 量子点/[Fe 2 S 2 (CO) 6] 复合材料是一种可持续且坚固的光催化剂，在三个循环后保持相同的活性。已经通过瞬态吸收 (TA) 和时间分辨光致发光 (TRPL) 光谱研究了 gC 3 N 4 /CdSe 量子点/[Fe 2 S 2 (CO) 6 ] 复合系统中的光致载流子转移动力学。分光结果表明从激发的CdSe量子点的价带有效的空穴转移到分子铁羰基簇和从量子点的缺陷状态到GC 3 Ñ 4中由GC 3 Ñ 4 / CdSe量子点/ [铁2秒2(CO) 6 ] 复合材料，可显着抑制 CdSe 量子点中光生载流子的复合，提高光催化活性和析氢稳定性。从 gC 3 N 4到 CdSe 量子点/[Fe 2 S 2 (CO) 6 ] 组件的能量转移，时间常数为 0.7 ns，也有助于电荷转移过程。
更新日期：2021-06-25
中文翻译：
用于增强光催化产氢的石墨氮化碳/CdSe量子点/羰基铁簇复合材料
成功构建了gC 3 N 4 /CdSe量子点/[Fe 2 S 2 (CO) 6 ]复合材料。复合材料的结构和化学成分尤其通过透射电子显微镜 (TEM)、傅里叶变换红外光谱 (FTIR) 和 X 射线光电子能谱 (XPS) 进行研究。研究了该组件作为质子还原形成氢气的光催化剂的能力。在可见光照射 4 小时后，gC 3 N 4 /CdSe 量子点/[Fe 2 S 2 (CO) 6催化的总 H 2生成] 复合材料被发现是相应的 CdSe/[Fe 2 S 2 (CO) 6 ] 组件的9 倍，并且显着高于单独的 CdSe 量子点或 gC 3 N 4。发现gC 3 N 4载体/基质在光催化析氢过程中提高了 CdSe 量子点/羰基铁簇组装的稳定性和效率。回收试验结果表明，gC 3 N 4 /CdSe 量子点/[Fe 2 S 2 (CO) 6] 复合材料是一种可持续且坚固的光催化剂，在三个循环后保持相同的活性。已经通过瞬态吸收 (TA) 和时间分辨光致发光 (TRPL) 光谱研究了 gC 3 N 4 /CdSe 量子点/[Fe 2 S 2 (CO) 6 ] 复合系统中的光致载流子转移动力学。分光结果表明从激发的CdSe量子点的价带有效的空穴转移到分子铁羰基簇和从量子点的缺陷状态到GC 3 Ñ 4中由GC 3 Ñ 4 / CdSe量子点/ [铁2秒2(CO) 6 ] 复合材料，可显着抑制 CdSe 量子点中光生载流子的复合，提高光催化活性和析氢稳定性。从 gC 3 N 4到 CdSe 量子点/[Fe 2 S 2 (CO) 6 ] 组件的能量转移，时间常数为 0.7 ns，也有助于电荷转移过程。
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