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Perylene Diimide Aggregates on Sb-Doped SnO2: Charge Transfer Dynamics Relevant to Solar Fuel Generation
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2017-08-16 00:00:00 , DOI: 10.1021/acs.jpcc.7b05928 Serena Berardi 1 , Vito Cristino 1 , Martina Canton 1 , Rita Boaretto 1 , Roberto Argazzi 1 , Elisabetta Benazzi 1 , Lucia Ganzer 2 , Rocío Borrego Varillas 2 , Giulio Cerullo 2 , Zois Syrgiannis 3 , Francesco Rigodanza 3 , Maurizio Prato 3, 4, 5 , Carlo Alberto Bignozzi 1 , Stefano Caramori 1
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2017-08-16 00:00:00 , DOI: 10.1021/acs.jpcc.7b05928 Serena Berardi 1 , Vito Cristino 1 , Martina Canton 1 , Rita Boaretto 1 , Roberto Argazzi 1 , Elisabetta Benazzi 1 , Lucia Ganzer 2 , Rocío Borrego Varillas 2 , Giulio Cerullo 2 , Zois Syrgiannis 3 , Francesco Rigodanza 3 , Maurizio Prato 3, 4, 5 , Carlo Alberto Bignozzi 1 , Stefano Caramori 1
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The deposition of perylene diimide-based aggregates (PDI) onto wide band gap n-type Sb-doped SnO2 (ATO) was investigated with the aim of finding efficient and versatile dye-sensitized platforms for photoelectrochemical solar fuel generation. These ATO-PDI photoanodes displayed hydrolytic stability in a wide range of pH (from 1 to 13) and revealed superior performances (up to 1 mA/cm2 net photocurrent at 1 V vs SCE) compared to both WO3-PDI and undoped SnO2-PDI when used in a photoelectrochemical setup for HBr splitting. Although ATO, SnO2, and WO3 are endowed with similar conduction band edge energetics, in ATO the presence of a significant density of intrabandgap states, whose occupancy varies with the applied potential, plays a substantial role in tuning the efficiency of photoinduced charge separation and collection. Furthermore, the investigation of the charge injection kinetics confirmed that, even in the absence of applied bias, ATO and WO3 are the best substrates for the oxidative quenching of poorly reducing PDI excited states, with at least a fraction of them injecting within <200 fs. The charge-separated states recombination occurs on longer time scales, allowing for their exploitation to drive demanding chemical reactions, as confirmed in photoelectrochemical water oxidation using IrO2-modified ATO-PDI photoanodes.
中文翻译：
ylene掺杂的SnO 2上的二亚胺聚集体：与太阳能发电相关的电荷转移动力学
研究了efficient二酰亚胺基团聚物（PDI）在宽带隙n型掺Sb的SnO 2（ATO ）上的沉积，目的是寻找高效，通用的染料敏化平台，用于光电化学太阳能燃料的生产。与WO 3 -PDI和未掺杂的SnO相比，这些ATO-PDI光阳极在宽范围的pH值（从1至13）中均显示出水解稳定性，并表现出卓越的性能（在1 V vs SCE下，高达1 mA / cm 2的净光电流）。在用于HBr分裂的光电化学装置中使用2 -PDI。尽管是ATO，SnO 2和WO 3由于具有相似的导带边缘能量，ATO中存在显着的带隙态密度，其占有率随施加的电势而变化，在调节光诱导电荷的分离和收集效率方面起着重要作用。此外，对电荷注入动力学的研究证实，即使在没有施加偏压的情况下，ATO和WO 3也是还原性较差的PDI激发态的氧化猝灭的最佳底物，其中至少有一部分在<200范围内注入fs。电荷分离的状态重组发生在更长的时间尺度上，从而允许它们的利用来驱动所需的化学反应，这在使用IrO 2修饰的ATO-PDI光电阳极的光电化学水氧化中得到了证实。
更新日期：2017-08-16
中文翻译：
ylene掺杂的SnO 2上的二亚胺聚集体：与太阳能发电相关的电荷转移动力学
研究了efficient二酰亚胺基团聚物（PDI）在宽带隙n型掺Sb的SnO 2（ATO ）上的沉积，目的是寻找高效，通用的染料敏化平台，用于光电化学太阳能燃料的生产。与WO 3 -PDI和未掺杂的SnO相比，这些ATO-PDI光阳极在宽范围的pH值（从1至13）中均显示出水解稳定性，并表现出卓越的性能（在1 V vs SCE下，高达1 mA / cm 2的净光电流）。在用于HBr分裂的光电化学装置中使用2 -PDI。尽管是ATO，SnO 2和WO 3由于具有相似的导带边缘能量，ATO中存在显着的带隙态密度，其占有率随施加的电势而变化，在调节光诱导电荷的分离和收集效率方面起着重要作用。此外，对电荷注入动力学的研究证实，即使在没有施加偏压的情况下，ATO和WO 3也是还原性较差的PDI激发态的氧化猝灭的最佳底物，其中至少有一部分在<200范围内注入fs。电荷分离的状态重组发生在更长的时间尺度上，从而允许它们的利用来驱动所需的化学反应，这在使用IrO 2修饰的ATO-PDI光电阳极的光电化学水氧化中得到了证实。
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