ZnO/D-A共轭聚合物S型异质结高效光催化产H2O2及其电荷转移动力学研究OA北大核心CSTPCD
Efficient Photocatalytic Production of H2O2 over ZnO/D-A Conjugated Polymer S-Scheme Heterojunction and Charge Transfer Dynamics Investigation
光催化技术利用清洁、无污染的太阳能合成过氧化氢(H2O2).本研究通过Suzuki Miiyaura反应和水热法合成了ZnO/PBD S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4.07 mmol∙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(H2O2).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 H2O2 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.
吴优;程畅;戚克振;程蓓;张建军;余家国;张留洋
大理大学药学院,云南 大理 671000||武汉理工大学,材料复合新技术国家重点实验室,武汉 430070武汉理工大学,材料复合新技术国家重点实验室,武汉 430070大理大学药学院,云南 大理 671000武汉理工大学,材料复合新技术国家重点实验室,武汉 430070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
化学
光催化产H2O2S型异质结ZnO缺陷态fs-TA光谱
Photocatalytic production of H2O2S-scheme heterojunctionZnO defect statesfs-TA spectroscopy
《物理化学学报》 2024 (11)
35-36,2
This work was supported by Yunnan Provincial Science and Technology Plan Project(202305AF150116)the National Natural Science Foundation of China(22238009,U23A20102,52073223,22278324 and 22361142704)the Natural Science Foundation of Hubei Province of China(2022CFA001).The project was also supported by the Fundamental Research Funds for the Central Universities,China University of Geosciences(Wuhan)(CUG22061). 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
评论