Disorder Engineering in Monolayer Nanosheets Enabling Photothermic Catalysis for Full Solar Spectrum (250–2500 nm) Harvesting

• Published in: Angewandte Chemie International Edition 2019-03, Vol.58 (10), p.3077-3081
• Main Authors: Yang, Min‐Quan, Shen, Lei, Lu, Yuyao, Chee, See Wee, Lu, Xin, Chi, Xiao, Chen, Zhihui, Xu, Qing‐Hua, Mirsaidov, Utkur, Ho, Ghim Wei
• Format: Article
• Language: English
• Subjects: Alternative energy sources; Catalysis; Catalysts; Combinatorial analysis; defect engineering; Electromagnetic absorption; Energy conversion; Fuel production; full solar spectrum; Incompatibility; Monolayers; Nanosheets; order–disorder; Photocatalysis; Photocatalysts; Photoexcitation; Photothermal conversion; photothermic catalysis; Photovoltaic cells; Purification; redox reaction; Solar heating; Water purification; Water treatment
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.201810694

A persistent challenge in classical photocatalyst systems with extended light absorption is the unavoidable trade‐off between maximizing light harvesting and sustaining high photoredox capability. Alternatively, cooperative energy conversion through photothermic activation and photocatalytic redox is a promising yet unmet scientific proposition that critically demands a spectrum‐tailored catalyst system. Here, we construct a solar thermal‐promoted photocatalyst, an ultrathin “biphasic” ordered–disordered D‐HNb3O8 junction, which performs two disparate spectral selective functions of photoexcitation by ordered structure and thermal activated conversion via disordered lattice for combinatorial photothermal mediated catalysis. This in situ synthetically immobilized lattice distortion, constrained to a single‐entity monolayer structure not only circumvents interfacial incompatibility but also triggers near‐field temperature rise at the catalyst–reactant complexes’ proximity to promote photoreaction. Ultimately, a generic full solar conversion improvement for H2 fuel production, organic transformation and water purification is realized. Let the sunshine in: Single‐entity ordered–disordered monolayer D‐HNb3O8 nanosheets were engineered to realize full solar spectrum (250–2500 nm) utilization. The crystalline domains absorb UV photons to generate charge carriers, while the disordered “nanoislands” capture the full spectrum for solar heating to thermally boost the reaction kinetics.