Jiang Chenfeng, Ding Yibo, Lin Jiayu, Sun Yi, Zhou Wei, Zhang Xiaoyan, Zhao Hongbin, Cao Weimin, Cheng Danhong
Department of Chemistry, College of Sciences, Shanghai University, Shanghai 200444, China.
Aerospace Hydrogen Energy (Shanghai) Technology Co., Ltd, Shanghai, 200241, China.
Dalton Trans. 2025 Feb 4;54(6):2460-2470. doi: 10.1039/d4dt03048f.
A TiO/CdS heterostructure has been widely investigated as a potential photoanode for photoelectrochemical (PEC) water splitting for hydrogen evolution. However, the efficiency and stability still remain challenging due to the sluggish reaction dynamics for water oxidation and easy photocorrosion of CdS. Here we report a ternary TiO/CdS/IrO heterostructure with IrO as a hole transport layer for PEC glycerol oxidation coupled with hydrogen evolution. The photocurrent density of the optimized TiO/CdS photoanode is 18.8 mA cm (1.23 V . RHE), which is about 10.6 times higher than that of the pristine TiO. It is found that most of the glycerol was converted to formic acid (FA) on the TiO/CdS surface with a production rate of ∼603.0 mmol m h. The average H production rate reaches 1574.5 mmol m h. After loading IrO nanoparticles, the products for glycerol oxidation remain unchanged with the production rate of FA reaching 863.4 mmol m h, while the hydrogen production rate is increased to 2345.2 mmol m h due to the improved stability. The results show that the obtained TiO/CdS/IrO heterostructure can effectively oxidize glycerol to value-added chemicals. The enhanced PEC performance and stability of the TiO/CdS/IrO photoanode can be ascribed to the greatly enhanced electrode/electrolyte interfacial carrier injection efficiency, caused by the fast glycerol oxidation dynamics and intimate contact. This work provides novel ideas to construct high-efficiency PEC systems for both clean energy production and high-value chemicals.
TiO/CdS异质结构作为一种用于光电化学（PEC）析氢水分解的潜在光阳极已得到广泛研究。然而，由于水氧化反应动力学缓慢以及CdS容易发生光腐蚀，其效率和稳定性仍然具有挑战性。在此，我们报道了一种三元TiO/CdS/IrO异质结构，其中IrO作为空穴传输层用于PEC甘油氧化并耦合析氢。优化后的TiO/CdS光阳极的光电流密度为18.8 mA cm²（1.23 V vs. RHE），约为原始TiO的10.6倍。研究发现，大部分甘油在TiO/CdS表面转化为甲酸（FA），生成速率约为603.0 mmol m⁻² h⁻¹。平均析氢速率达到1574.5 mmol m⁻² h⁻¹。负载IrO纳米颗粒后，甘油氧化产物保持不变，FA生成速率达到863.4 mmol m⁻² h⁻¹，而由于稳定性提高，析氢速率增加到2345.2 mmol m⁻² h⁻¹。结果表明，所获得的TiO/CdS/IrO异质结构能够有效地将甘油氧化为增值化学品。TiO/CdS/IrO光阳极PEC性能和稳定性的增强可归因于快速的甘油氧化动力学和紧密接触导致的电极/电解质界面载流子注入效率的大幅提高。这项工作为构建用于清洁能源生产和高价值化学品的高效PEC系统提供了新思路。
