半菁染料作为染料敏化太阳能电池吸光材料的理论研究

引用本文: 李会学, 左国防, 李志锋, 王晓峰, 郑仁慧. 半菁染料作为染料敏化太阳能电池吸光材料的理论研究[J]. 物理化学学报, 2015, 31(5): 866-876. doi: 10.3866/PKU.WHXB201503254 shu

Citation: LI Hui-Xue, ZUO Guo-Fang, LI Zhi-Feng, WANG Xiao-Feng, ZHENG Ren-Hui. Theoretical Study of Hemicyanine Dye as a Dye-Sensitized Solar Cell Light-Absorbing Material[J]. Acta Physico-Chimica Sinica, 2015, 31(5): 866-876. doi: 10.3866/PKU.WHXB201503254 shu

半菁染料作为染料敏化太阳能电池吸光材料的理论研究

基金项目:
国家自然科学基金(21465021, 21463023) (21465021, 21463023)

教育部重点项目(211189) (211189)

甘肃省自然科学基金(1208RJZE139) (1208RJZE139)

甘肃省高校领军人才项目(11zx-04)资助 (11zx-04)

摘要:

采用第一性原理研究了半菁-二氧化钛团簇形成的配合物(hemicyanine-(TiO₂)_n)的光电子转移过程, 这里n分别取5, 9, 15. 配合物基态构型采用密度泛函理论方法进行优化, 而激发态采用含时密度泛函理论进行计算. 采用长程相关校正的密度泛函CAM-B3LYP和ωB97X-D计算的激发能与实验值吻合得很好. 依据广义Mulliken-Hush (GMH)公式, 基于密度泛函理论得到的波函数被用来计算电荷转移积分, 进而可根据Marcus理论计算出电荷分离速率常数(k_CS)和电荷回传速率常数(k_CR). 计算结果表明电子从染料到(TiO₂)_n团簇的传递有多条通道, 这使得k_CS具有更大值, 相反, 只具有单通道的电荷回传降低了k_CR值, 与k_CS相比甚至可以忽略, 这表明在所研究的体系中电荷回传是不利的.

关键词:

English

Theoretical Study of Hemicyanine Dye as a Dye-Sensitized Solar Cell Light-Absorbing Material

1.
1 College of Chemical Engineering and Technology, Tianshui Normal University, Tianshui 741001, Gansu Province, P. R. China;
2 State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China
Received Date: 27 February 2015
Available Online: 08 May 2015
Fund Project:
国家自然科学基金(21465021, 21463023)

教育部重点项目(211189)

甘肃省自然科学基金(1208RJZE139)

甘肃省高校领军人才项目(11zx-04)资助

Abstract:

We used first-principles calculations to investigate the photo-induced electron transfer (PIET) process of the hemicyanine-(TiO₂)_n complex ((TiO₂)_n-dye) for n=5, 9, 15. The geometries of the (TiO₂)_n-dye in the ground state were optimized using density functional theory (DFT) and their excited states were investigated using the time-dependent DFT (TDDFT) method. The excited energies, which were calculated using the longrange- corrected functionals, CAM-B3LYP and ωB97X-D, were in od agreement with the experimentally observed values. The wave functions based on DFT were used to calculate the charge transfer integrals by the generalized Mulliken-Hush (GMH) approach. In addition, the photo-induced charge separation rate constant (k_CS) and charge recombination rate constant (k_CR) were calculated using Marcus theory. The calculated results showed that there were a cascade of electron transfer channels from the dye into the (TiO₂)_n cluster, which increases the k_CS value. In contrast, the single channel of charge recombination decreases the k_CR value, which is negligible compared with k_CS, indicating that electron recombination is not favored.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

半菁染料作为染料敏化太阳能电池吸光材料的理论研究

English

Theoretical Study of Hemicyanine Dye as a Dye-Sensitized Solar Cell Light-Absorbing Material

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

半菁染料作为染料敏化太阳能电池吸光材料的理论研究

English

Theoretical Study of Hemicyanine Dye as a Dye-Sensitized Solar Cell Light-Absorbing Material

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

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