Disorder Engineering in Monolayer Nanosheets Enabling Photothermic Catalysis for Full Solar Spectrum (250-2500 nm) Harvesting.
Disorder Engineering in Monolayer Nanosheets Enabling Photothermic Catalysis for Full Solar Spectrum (250-2500 nm) Harvesting.
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DOI：
10.1002/anie.201810694
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发表时间：
2019-03
影响因子：
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通讯作者：
Min‐Quan Yang;Lei Shen;Yuyao Lu;S. Chee;Xin Lu;X. Chi;Zhihui Chen;Qinghua Xu;U. Mirsaidov
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文献类型：
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作者：
Min‐Quan Yang;Lei Shen;Yuyao Lu;S. Chee;Xin Lu;X. Chi;Zhihui Chen;Qinghua Xu;U. Mirsaidov
在具有扩展光吸收的经典光催化剂系统中，一个持续的挑战是在最大化光捕获和保持高光氧化还原能力之间不可避免地权衡。或者，通过光热活化和光催化氧化还原来协同能量转换是一个很有前途但尚未得到满足的科学命题，这一命题迫切需要一个针对光谱定制的催化剂系统。在这里，我们构建了一种太阳能热促进光催化剂，一种超薄的有序-无序D-HNb3O8结，它具有两种不同的光谱选择功能，即有序结构的光激发和无序晶格的热激活转化，用于组合光热催化。这种原位合成固定的晶格扭曲被限制在单一实体的单分子结构中，不仅绕过了界面不相容，而且在催化剂-反应物复合体附近触发近场温度升高，以促进光反应。最终，实现了氢气燃料生产、有机转化和水净化的通用全太阳能转换改进。
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-HNb3 O8 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.