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DOE OSTI · 3363742

A photochargeable semiconductor for highly efficient dehydrogenative coupling of amines

Luo, Jie [University of California, Berkeley, CA (United States); BASF Corporation, Berkeley, CA (United States)] (ORCID:000900015256644X)·Chen, Xinyu [University of California, Berkeley, CA (United States); BASF Corporation, Berkeley, CA (United States)]·Jayasinghe, Lihini [University of California, Berkeley, CA (United States)] (ORCID:0000000284500728)·Soland, Nathan Edward [University of California, Berkeley, CA (United States)]·Shan, Yu [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000281658407)·Maulana, Arifin Luthfi [BASF Corporation, Berkeley, CA (United States); University of California, Berkeley, CA (United States)] (ORCID:000000025928586X)·Zhu, Heqing [University of California, Berkeley, CA (United States)] (ORCID:0009000205790972)·Guzman, Maria Fonseca [University of California, Berkeley, CA (United States)]·Oddo, Alexander M. [University of California, Berkeley, CA (United States)] (ORCID:0000000254588650)·Donnelly, Kiran M. [University of California, Berkeley, CA (United States)] (ORCID:0009000063137328)·Choi, Jihoon [University of California, Berkeley, CA (United States)] (ORCID:0000000273113087)·Feijoo, Julian [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]·Schaefer, Bernd [BASF Corporation (Germany)] (ORCID:0000000217359795)·Schmalzbauer, Matthias [BASF Corporation (Germany)] (ORCID:0000000265192184)·Zhang, Rui [BASF Corporation, Berkeley, CA (United States)]·Seeler, Fabian [BASF Corporation (Germany)]·Lizandara-Pueyo, Carlos [BASF Corporation, Berkeley, CA (United States); BASF Corporation (Germany)] (ORCID:000000031146775X)·Schaller, Richard D. [Northwestern Univ., Evanston, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)] (ORCID:0000000196968830)·Yang, Peidong [University of California, Berkeley, CA (United States); BASF Corporation, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000347991684)
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Abstract

The development of materials with high photocatalytic efficiency is essential for sustainable chemical transformations. Here, in this work, we introduce photochargeable zinc indium sulfide nanocrystals with notable charge storage capacity, enabling highly efficient photocatalytic dehydrogenative coupling of amines. Combined with a nickel cocatalyst, the nanocrystals deliver diamines and hydrogen at rates exceeding 120 mmol per gram of photocatalyst per hour, with > 95% selectivity and an apparent quantum efficiency of up to 39.4% under ambient conditions. The system exhibits excellent scalability, demonstrated by a reaction on a 20-g scale, and broad versatility in promoting amino acid ester coupling and polymerization reactions with concurrent hydrogen evolution. Mechanistic studies attribute the photocharging capability of zinc indium sulfide nanocrystals to in situ-generated trap states such as sulfur vacancies, which extend hydrogen production into the dark catalytic cycle and enhance the overall charge utilization efficiency. These findings position photochargeable semiconductors as promising platforms for a wide range of photocatalytic applications.

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Luo, Jie [University of California, Berkeley, CA (United States); BASF Corporation, Berkeley, CA (United States)] (ORCID:000900015256644X), Chen, Xinyu [University of California, Berkeley, CA (United States); BASF Corporation, Berkeley, CA (United States)], Jayasinghe, Lihini [University of California, Berkeley, CA (United States)] (ORCID:0000000284500728), Soland, Nathan Edward [University of California, Berkeley, CA (United States)], Shan, Yu [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000281658407), Maulana, Arifin Luthfi [BASF Corporation, Berkeley, CA (United States); University of California, Berkeley, CA (United States)] (ORCID:000000025928586X), Zhu, Heqing [University of California, Berkeley, CA (United States)] (ORCID:0009000205790972), Guzman, Maria Fonseca [University of California, Berkeley, CA (United States)], Oddo, Alexander M. [University of California, Berkeley, CA (United States)] (ORCID:0000000254588650), Donnelly, Kiran M. [University of California, Berkeley, CA (United States)] (ORCID:0009000063137328), Choi, Jihoon [University of California, Berkeley, CA (United States)] (ORCID:0000000273113087), Feijoo, Julian [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Schaefer, Bernd [BASF Corporation (Germany)] (ORCID:0000000217359795), Schmalzbauer, Matthias [BASF Corporation (Germany)] (ORCID:0000000265192184), Zhang, Rui [BASF Corporation, Berkeley, CA (United States)], Seeler, Fabian [BASF Corporation (Germany)], Lizandara-Pueyo, Carlos [BASF Corporation, Berkeley, CA (United States); BASF Corporation (Germany)] (ORCID:000000031146775X), Schaller, Richard D. [Northwestern Univ., Evanston, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)] (ORCID:0000000196968830), Yang, Peidong [University of California, Berkeley, CA (United States); BASF Corporation, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000347991684). 2026-03-30. A photochargeable semiconductor for highly efficient dehydrogenative coupling of amines. https://doi.org/10.1038/s41557-026-02109-6

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