journal article·2022-12-07

Inductive Effect of Lewis Acidic Dopants on the Band Levels of Perovskite for a Photocatalytic Reaction

Yunhee Cho, Hyojung Kim, Sanggil Lee, Eunji Lee, Yosep Hwang, Hyunjung Kim, Sohyeon Seo, Ngoc Quang Tran, Won Bin Kim, Hyun Suk Jung, Jeongyong Kim, Mun Seok Jeong, Hyoyoung Lee

ACS Applied Materials & Interfaces· Volume 14· Issue 48
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Abstract

Band-edge modulation of halide perovskites as photoabsorbers plays significant roles in the application of photovoltaic and photochemical systems. Here, Lewis acidity of dopants (M) as the new descriptor of engineering the band-edge position of the perovskite is investigated in the gradiently doped perovskite along the core-to-surface (CsPbBr3–CsPb1–xMxBr3). Reducing M–bromide bond strength with an increase in hardness of acidic M increases the electron ability of basic Br, thus strengthening the Pb–Br orbital coupling in M–Pb–Br, noted as the inductive effect of dopants. Especially, the highly hard Lewis acidic Mg localized in the outer position of the perovskite induces the increase of work function and then shifts band edge upward along the core-to-surface of the perovskite. Thus, charge separation driven by the dopant-induced internal electric field induces the slow annihilation of the excited holes, improving the slow aromatic Csp3–H dissociation in the photocatalytic oxidation process by ∼211% (491.39 μmol g–1 h–1) enhancements, compared with undoped nanocrystals.
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Research context

OpenAlex topics: Perovskite Materials and Applications · Solid-state spectroscopy and crystallography · Quantum Dots Synthesis And Properties

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Chemistry, Sungkyunkwan University (SKKU), Suwon16419, Republic of Korea

Center for Integrated Nanostructure Physics (CINAP), Institute for Basic Science (IBS), Sungkyunkwan University (SKKU), Suwon16419, Republic of Korea

Artificial Atom and Quantum Materials Center, Sungkyunkwan University (SKKU), Suwon16419, Republic of Korea

Center for Research Equipment, Division of Scientific Instrumentation & Management, Korea Basic Science Institute, Gwahak-ro, Yuseong-gu, Daejeon34133, Republic of Korea

Department of Energy Science, Sungkyunkwan University (SKKU), Suwon16419, Republic of Korea

Creative Research Institute, Sungkyunkwan University (SKKU), Suwon16419, Republic of Korea

School of Advanced Materials Science and Engineering, Sungkyunkwan University (SKKU), Suwon16419, Republic of Korea

Department of Energy Engineering, Hanyang University, Seoul04763, Republic of Korea

Department of Biophysics, Sungkyunkwan University (SKKU), Suwon16419, Republic of Korea

Funding

National Research Foundation of Korea · Korea Medical Device Development Fund · Institute for Basic Science · Korea Evaluation Institute of Industrial Technology · Scale-up Support Program for Environmental Small-Medium Enterpris

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