ZnO/D-A共轭聚合物S型异质结高效光催化产H_(2)O_(2)及其电荷转移动力学研究  

Efficient Photocatalytic Production of H_(2)O_(2) over ZnO/D-A Conjugated Polymer S-Scheme Heterojunction and Charge Transfer Dynamics Investigation

作　　者：吴优 程畅 戚克振 程蓓[2] 张建军 余家国 张留洋 You Wu;Chang Cheng;Kezhen Qi;Bei Cheng;Jianjun Zhang;Jiaguo Yu;Liuyang Zhang(College of Pharmacy,Dali University,Dali 671000,Yunnan Province,China;State Key Laboratory of Advanced Technology for Materials Synthesis and Processing,Wuhan University of Technology,Wuhan 430070,China;Laboratory of Solar Fuel,Faculty of Materials Science and Chemistry,China University of Geosciences,Wuhan 430078,China)

机构地区：[1]大理大学药学院,云南大理671000 [2]武汉理工大学,材料复合新技术国家重点实验室,武汉430070 [3]中国地质大学(武汉),材料与化学学院太阳燃料实验室,武汉430078

出　　处：《物理化学学报》2024年第11期35-36,共2页Acta Physico-Chimica Sinica

基　　金：云南省科技计划项目(202305AF150116);国家自然科学基金(22238009,U23A20102,52073223,22278324和22361142704);湖北省自然科学基金(2022CFA001);中国地质大学(武汉)中央高校基本科研业务费(CUG22061)的支持。

摘　　要：光催化技术利用清洁、无污染的太阳能合成过氧化氢(H_(2)O_(2))。本研究通过SuzukiMiiyaura反应和水热法合成了ZnO/PBDS型异质结复合材料。优化后的ZnO/PBD复合材料的光催化产H2O2效率为4.07mmol·g^(-1)·h^(-1),是单一ZnO的5.4倍。光催化性能的显著提高归功于S型异质结的形成。紫外可见吸收光谱和原位光照X射线光电子能谱证实了S型异质结的形成。稳态荧光和飞秒瞬态吸收(fs-TA)光谱确定并验证了ZnO中缺陷态的存在。这些缺陷态会捕获光生电子,不利于光催化反应。S型异质结有效地促进了电子的分离和转移,从而缓解了这一问题。通过拟合fs-TA光谱得到了光生电子在这些缺陷态中的寿命,进一步证明了S型异质结中的载流子转移机制。该工作介绍了一种利用fs-TA光谱研究有机/无机S型异质结的新方法。Photocatalytic technology harnesses clean,non-polluting solar energy to synthesize hydrogen peroxide(H_(2)O_(2)).In this study,ZnO/PBD S-scheme heterojunction composites,featuring ZnO nanoparticles on a donor-acceptor conjugated polymer substrate(PBD),were synthesized via the Suzuki-Miyaura reaction and hydrothermal method.The optimal ZnO/PBD composite achieved an H_(2)O_(2) production efficiency of 4.07 mmol·g^(-1)·h^(-1),which is 5.4 times higher than that of pristine ZnO.This significant enhancement is attributed to the formation of S-scheme heterojunctions.The successful construction of S-scheme heterojunctions was confirmed through UV-visible absorption spectroscopy and in situ irradiated X-ray photoelectron spectroscopy.Steady-state photoluminescence and femtosecond transient absorption(fs-TA)spectroscopies identified and verified the presence of defect states in ZnO.These defect states trap photogenerated electrons,adversely affecting the photocatalytic reaction.However,the S-scheme heterojunction effectively promotes the separation and transfer of electrons,mitigating this issue.The measured lifetimes of photogenerated electrons in these defect states,as determined by fitted fs-TA decay kinetics,provided further evidence of the carrier transfer mechanism in S-scheme heterojunctions.This work introduces a novel approach for studying organic/inorganic S-scheme heterojunctions using fs-TA spectroscopy.

关 键 词：光催化产H_(2)O_(2) S型异质结 ZnO缺陷态 fs-TA光谱 

分 类 号：O643[理学—物理化学]