Generation of long-lived charges in organic semiconductor heterojunction nanoparticles for efficient photocatalytic hydrogen evolution

Jan Kosco (), Soranyel Gonzalez-Carrero, Calvyn T. Howells, Teng Fei, Yifan Dong, Rachid Sougrat, George T. Harrison, Yuliar Firdaus, Rajendar Sheelamanthula, Balaji Purushothaman, Floriana Moruzzi, Weidong Xu, Lingyun Zhao, Aniruddha Basu, Stefaan De Wolf, Thomas D. Anthopoulos, James R. Durrant () and Iain McCulloch ()
Additional contact information
Jan Kosco: King Abdullah University of Science and Technology (KAUST), KAUST Solar Center (KSC), Physical Sciences and Engineering Division (PSE)
Soranyel Gonzalez-Carrero: Imperial College London
Calvyn T. Howells: King Abdullah University of Science and Technology (KAUST), KAUST Solar Center (KSC), Physical Sciences and Engineering Division (PSE)
Teng Fei: Imperial College London
Yifan Dong: Imperial College London
Rachid Sougrat: KAUST Core Labs, King Abdullah University of Science and Technology (KAUST)
George T. Harrison: King Abdullah University of Science and Technology (KAUST), KAUST Solar Center (KSC), Physical Sciences and Engineering Division (PSE)
Yuliar Firdaus: King Abdullah University of Science and Technology (KAUST), KAUST Solar Center (KSC), Physical Sciences and Engineering Division (PSE)
Rajendar Sheelamanthula: King Abdullah University of Science and Technology (KAUST), KAUST Solar Center (KSC), Physical Sciences and Engineering Division (PSE)
Balaji Purushothaman: King Abdullah University of Science and Technology (KAUST), KAUST Solar Center (KSC), Physical Sciences and Engineering Division (PSE)
Floriana Moruzzi: University of Oxford
Weidong Xu: Imperial College London
Lingyun Zhao: KAUST Core Labs, King Abdullah University of Science and Technology (KAUST)
Aniruddha Basu: King Abdullah University of Science and Technology (KAUST), KAUST Solar Center (KSC), Physical Sciences and Engineering Division (PSE)
Stefaan De Wolf: King Abdullah University of Science and Technology (KAUST), KAUST Solar Center (KSC), Physical Sciences and Engineering Division (PSE)
Thomas D. Anthopoulos: King Abdullah University of Science and Technology (KAUST), KAUST Solar Center (KSC), Physical Sciences and Engineering Division (PSE)
James R. Durrant: Imperial College London
Iain McCulloch: King Abdullah University of Science and Technology (KAUST), KAUST Solar Center (KSC), Physical Sciences and Engineering Division (PSE)

Nature Energy, 2022, vol. 7, issue 4, 340-351

Abstract: Abstract Organic semiconductor photocatalysts for the production of solar fuels are attractive as they can be synthetically tuned to absorb visible light while simultaneously retaining suitable energy levels to drive a range of processes. However, a greater understanding of the photophysics that determines the function of organic semiconductor heterojunction nanoparticles is needed to optimize performance. Here, we show that such materials can intrinsically generate remarkably long-lived reactive charges, enabling them to efficiently drive sacrificial hydrogen evolution. Our optimized hetereojunction photocatalysts comprise the conjugated polymer PM6 matched with Y6 or PCBM electron acceptors, and achieve external quantum efficiencies of 1.0% to 5.0% at 400 to 900 nm and 8.7% to 2.6% at 400 to 700 nm, respectively. Employing transient and operando spectroscopies, we find that the heterojunction structure in these nanoparticles greatly enhances the generation of long-lived charges (millisecond to second timescale) even in the absence of electron/hole scavengers or Pt. Such long-lived reactive charges open potential applications in water-splitting Z-schemes and in driving kinetically slow and technologically desirable oxidations.

Date: 2022
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DOI: 10.1038/s41560-022-00990-2

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