Journal
SMALL
Volume 16, Issue 40, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202001752
Keywords
charge separation; oxygen vacancy; porphyrin; reverse regulation
Categories
Funding
- Natural Science Foundation of China [21575115, 21705117]
- Program for Chang Jiang Scholars and Innovative Research Team, Ministry of Education, China [IRT-16R61]
- Program of Gansu Provincial Higher Education Research Project [2017-D-01]
- Program of Tianjin Science and Technology Major Project and Engineering [19ZXYXSY00090]
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Highly efficient charge separation has been demonstrated as one of the most significant steps playing decisive roles in enhancing the overall efficiency of photoelectrochemical (PEC) processes. In this study, by employing 5,10,15,20-tetrakis (4-carboxyphenyl) porphyrin-Ni (NiTCPP) as a prototype, an oxygen vacancy (Vo)-mediated reverse regulation strategy is proposed for tuning hole transfer, which in turn can accelerate the transport of electrons and thus enhancing charge separation. The optimal NiO/NiTCPP system exhibits much higher (approximate to 40 times) photocurrent and longer (approximate to 13 times) lifetime of charge carriers compared with those of pure NiTCPP. Furthermore, the electron transfer kinetic rate constant (K-eff) is quantitatively determined by an efficient scanning photoelectrochemical microscopy (SPECM). TheK(eff)of the optimal system has a 5.7-fold improvement. In addition, the similar enhancement in charge separation from other semiconductors (CoTCPP and FeTCPP) are also observed, indicating that the Vo-mediated reverse regulation strategy is a promising pathway for tuning the properties of light harvesters in solar energy conversion.
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