Bifunctional g-C3N4 nanospheres/CdZnS QDs S-scheme photocatalyst with boosted H2 evolution and furfural synthesis mechanism

Guotai Sun, Zige Tai, Jianjun Zhang, Bei Cheng, Huogen Yu, Jiaguo Yu
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Abstract

Photocatalytic H evolution coupled with organic oxidation could replace the slow four-electron water oxidation and utilize charge carriers to obtain high-valued chemicals. Herein, inorganic CdZnS quantum dots (QDs) are skillfully deposited on g-CN nanospheres to construct an inorganic-polymeric S-scheme heterostructure. The CN-CdZnS photocatalyst presents enhanced light absorption, abundant active sites, and intimate interface contact. The optimized composite exhibits an enhanced H evolution rate of 582.3 μmol/g/h and a furfuryl alcohol (FAL) conversion of 84.2 %. Femtosecond transient absorption (fs-TA) spectroscopy, irradiation X-ray photoelectron spectroscopy (XPS), electron paramagnetic resonance (EPR), and theoretical calculation (DFT) verify the S-scheme mechanism, which promotes charge separation and strengthens carrier redox ability. infrared spectra reveal that FAL is first activated to CHO radical by holes in CdZnS and further oxidized to furfural (FF) with dehydrogenation of its hydroxyl group. This work supplies new insight into designing efficient photocatalysts for H generation and organic synthesis.
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具有促进 H2 演化和糠醛合成机制的 g-C3N4 纳米球/CdZnS QDs S 型双功能光催化剂
光催化氢进化与有机物氧化相结合,可以取代缓慢的四电子水氧化,并利用电荷载流子获得高价值的化学物质。在这里,无机 CdZnS 量子点(QDs)被巧妙地沉积在 g-CN 纳米球上,从而构建了一种无机聚合物 S 型异质结构。CN-CdZnS 光催化剂具有更强的光吸收能力、丰富的活性位点和亲密的界面接触。优化后的复合材料表现出更高的 H 演化率(582.3 μmol/g/h)和 84.2% 的糠醇(FAL)转化率。飞秒瞬态吸收 (fs-TA) 光谱、辐照 X 射线光电子能谱 (XPS)、电子顺磁共振 (EPR) 和理论计算 (DFT) 验证了促进电荷分离和增强载体氧化还原能力的 S 型机制。这项研究为设计高效的光催化剂用于氢气生成和有机合成提供了新的视角。
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