Authors
Dongyang Li, Fanyu Meng, Shaohua Xiao, Wenyan Dan, Chao Wu, Xingwang Lan, Chi Zhang, Honghan Fei
Published in
Angewandte Chemie (International ed. in English). Oct 21, 2026. Epub Oct 21, 2026.
Abstract
Two-dimensional (2D) lead halides provide a versatile platform for interlayer engineering, but their functionality is limited by electronically inert spacers. The integration of electronically active inorganic motifs into layered lead halide lattices remains a major challenge. Herein, we report a coordination-directed strategy that enables the programmable incorporation of transition-metal-sulfur (MS2) units into layered lead halides via synergistic carboxylate-sulfide dual binding, affording a family of 12 crystalline frameworks with tunable compositions. Embedding electronically and catalytically active MS2 motifs transforms the interlayer region from a passive dielectric component into an active domain for charge transport and catalysis. Notably, CoS2- and NiS2-intercalated lead-halide materials exhibit efficient CO2-to-CO conversion, achieving rates up to 4.32 mmol g-1 h-1, an apparent quantum yield of 1.76%, and near-unity selectivity. Combined in situ spectroscopy and density functional theory calculations identify NiS2 as the optimal catalytic center, featuring favorable band alignment, efficient charge transfer, and moderate CO adsorption. In contrast, the FeS2-intercalated material suffers from catalyst poisoning due to strong CO binding, while MnS2-, ZnS2-, and CuS2-based systems are limited by unfavorable energy alignment with the photosensitizer or competing self-reduction pathways. This work introduces a new paradigm that integrates efficient light-harvesting, charge transport, and catalytic functionality within a single layered semiconductor.
PMID:
42908067
Bibliographic data and abstract were imported from PubMed on 23 Oct 2026.
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