Hierarchically Periodic Macroporous CdS–ZnO Heterojunctions with Multiple Quantum Well-like Band Alignments for Efficient Photocatalytic Hydrogen Evolution without a Cocatalyst,ACS Sustainable Chemistry & Engineering

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Hierarchically Periodic Macroporous CdS–ZnO Heterojunctions with Multiple Quantum Well-like Band Alignments for Efficient Photocatalytic Hydrogen Evolution without a Cocatalyst
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2023-02-08 , DOI: 10.1021/acssuschemeng.2c07255
Qingzhuo Lin ₁ , Shudong Liang ₁ , Jintao Wang ₁ , Rongbin Zhang ₁ , Gang Liu _{2,

3} , Xuewen Wang ₁

Affiliation

Heterostructures constructed by conventional methods, particularly those randomly distributed manner on the catalyst surface as well as forming core–shell structures, lead to imbalance in carrier utilization, limitation of charge extraction/transfer, and hindrance of light harvesting. In this study, we constructed a new type of heterostructure consisting of alternate CdS and ZnO grains bridged with good interfaces in the hierarchically periodic macroporous (HPM) walls by the pyrolysis of CdZnS solid solution in a polymethyl methacrylate nanoreactor. Since the alternately arranged CdS–ZnO heterojunctions in the HPM form multiple quantum well-like (MQW-like) band alignments that favor the Z-scheme charge transfer, the photogenerated electrons and holes are spatially separate and accumulated on CdS and ZnO parts, respectively. Besides the desirable spatial separation of the photogenerated charges, the enabled excellent mass transfer in the macroporous structures effectively accelerates the utilization of the carriers. Owing to the synergistic effect of the MQW-like band alignments and the HPM structures, the photocatalytic H₂ evolution rate of HPM CdS–ZnO is as high as 587.8 μmol h^–1 without a cocatalyst. This work introduces a fascinating strategy for the creation of alternate heterojunctions to improve carrier utilization.

中文翻译：

多级周期性大孔 CdS-ZnO 异质结与多量子阱状带排列，用于在没有助催化剂的情况下进行高效光催化析氢

通过传统方法构建的异质结构，特别是那些随机分布在催化剂表面以及形成核壳结构的异质结构，会导致载流子利用不平衡、电荷提取/转移受限以及光捕获受阻。在这项研究中，我们通过 CdZnS 固溶体在聚甲基丙烯酸甲酯纳米反应器中的热解，构建了一种新型异质结构，该异质结构由交替的 CdS 和 ZnO 晶粒桥接在分级周期性大孔 (HPM) 壁中的良好界面。由于 HPM 中交替排列的 CdS-ZnO 异质结形成有利于 Z 型电荷转移的多量子阱状（MQW 状）带排列，因此光生电子和空穴在空间上分离并分别累积在 CdS 和 ZnO 部分上. 除了光生电荷的理想空间分离外，大孔结构中出色的质量传递有效地加速了载流子的利用。由于类 MQW 带排列和 HPM 结构的协同作用，光催化 H₂在没有助催化剂的情况下，HPM CdS–ZnO 的析出速率高达 587.8 μmol h ^{–1 。}这项工作介绍了一种用于创建交替异质结以提高载流子利用率的迷人策略。

更新日期：2023-02-08

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