Omnidirectional Hydrogen Generation Based on a Flexible Black Gold Nanotube Array.

Solar-driven hydrogen generation is emerging as an economical and sustainable means of producing renewable energy. However, current photocatalysts for hydrogen generation are mostly powder-based or rigid-substrate-supported, which suffer from limitations, such as difficulties in catalyst regeneration or poor omnidirectional light-harvesting. Here, we report a two-dimensional (2D) flexible photocatalyst based on elastomer-supported black gold nanotube (GNT) arrays with conformal CdS coating and Pt decoration. The highly porous GNT arrays display a strong light-trapping effect, leading to near-complete absorption over almost the entire range of the solar spectrum. In addition, they offer high surface-to-volume ratios promoting efficient photocatalytic reactions. These structural features result in high H2 generation efficiencies. Importantly, our elastomer-supported photocatalyst displays comparable photocatalytic activity even when being mechanically deformed, including bending, stretching, and twisting. We further designed a three-dimensional (3D) tree-like flexible photocatalytic system to mimic Nature's photosynthesis, which demonstrated omnidirectional H2 generation. We believe our strategy represents a promising route in designing next-generation solar-to-fuel systems that rival natural plants.

[1]  Wee‐Jun Ong,et al.  Shining light on ZnIn 2 S 4 photocatalysts: Promotional effects of surface and heterostructure engineering toward artificial photosynthesis , 2022, EcoMat.

[2]  Wenlong Cheng,et al.  Fine‐Tuning Au@Pd Nanocrystals for Maximum Plasmon‐Enhanced Catalysis , 2020, Advanced Materials Interfaces.

[3]  K. Domen,et al.  Visible-Light-Driven Photocatalytic Water Splitting: Recent Progress and Challenges , 2020 .

[4]  V. Svorcik,et al.  Plasmon-induced water splitting - through flexible hybrid 2D architecture up to hydrogen from seawater under NIR light. , 2020, ACS applied materials & interfaces.

[5]  Yueping Fang,et al.  Bio-inspired multilayered graphene-directed assembly of monolithic photo-membrane for full-visible light response and efficient charge separation , 2020 .

[6]  V. A. Apkarian,et al.  Efficient Plasmon-Mediated Energy Funneling to the Surface of Au@Pt Core-Shell Nanocrystals. , 2020, ACS nano.

[7]  Rongshu Zhu,et al.  Leaf-inspired structural design of artificial leaf BiVO4/InVO4 heterojunction with enhanced photocatalytic activity for pollutant degradation , 2020 .

[8]  Fang‐Xing Xiao,et al.  Partially Self-Transformed Transition-Metal Chalcogenide Interim Layer: Motivating Charge Transport Cascade for Solar Hydrogen Evolution. , 2020, Inorganic chemistry.

[9]  K. Domen,et al.  Particulate Photocatalysts for Light-Driven Water Splitting: Mechanisms, Challenges, and Design Strategies. , 2020, Chemical reviews.

[10]  Jeong Y. Park,et al.  Plasmon‐Induced Hot Carrier Separation across Dual Interface in Gold–Nickel Phosphide Heterojunction for Photocatalytic Water Splitting , 2019, Advanced Functional Materials.

[11]  L. Besteiro,et al.  Applications of Plasmon-Enhanced Nanocatalysis to Organic Transformations. , 2019, Chemical reviews.

[12]  Wenxiang Zhang,et al.  Collective excitation of plasmon-coupled Au-nanochain boosts photocatalytic hydrogen evolution of semiconductor , 2019, Nature Communications.

[13]  Z. Suo,et al.  Giant Poisson's Effect for Wrinkle‐Free Stretchable Transparent Electrodes , 2019, Advanced materials.

[14]  M. Xu,et al.  Efficient Plasmonic Au/CdSe Nanodumbbell for Photoelectrochemical Hydrogen Generation beyond Visible Region , 2019, Advanced Energy Materials.

[15]  H. Misawa,et al.  Enhanced water splitting under modal strong coupling conditions , 2018, Nature Nanotechnology.

[16]  Zhenyi Zhang,et al.  UV‐Vis‐NIR‐Driven Plasmonic Photocatalysts with Dual‐Resonance Modes for Synergistically Enhancing H2 Generation , 2018 .

[17]  Tsuyoshi Takata,et al.  A Particulate Photocatalyst Water-Splitting Panel for Large-Scale Solar Hydrogen Generation , 2018 .

[18]  H. Tada,et al.  Red-Light-Driven Water Splitting by Au(Core)-CdS(Shell) Half-Cut Nanoegg with Heteroepitaxial Junction. , 2018, Journal of the American Chemical Society.

[19]  Wenxiao Guo,et al.  Surface-Plasmon-Driven Hot Electron Photochemistry. , 2017, Chemical reviews.

[20]  K. Domen,et al.  Particulate photocatalysts for overall water splitting , 2017 .

[21]  C. Tung,et al.  Self‐Assembled Au/CdSe Nanocrystal Clusters for Plasmon‐Mediated Photocatalytic Hydrogen Evolution , 2017, Advanced materials.

[22]  K. Domen,et al.  Photocatalyst Sheets Composed of Particulate LaMg1/3Ta2/3O2N and Mo-Doped BiVO4 for Z-Scheme Water Splitting under Visible Light , 2016 .

[23]  Bugra Turan,et al.  Upscaling of integrated photoelectrochemical water-splitting devices to large areas , 2016, Nature Communications.

[24]  Ququan Wang,et al.  Improved Hydrogen Production of Au–Pt–CdS Hetero‐Nanostructures by Efficient Plasmon‐Induced Multipathway Electron Transfer , 2016 .

[25]  Bin Zhu,et al.  Self-assembly of highly efficient, broadband plasmonic absorbers for solar steam generation , 2016, Science Advances.

[26]  W. Cai,et al.  Black Gold: Plasmonic Colloidosomes with Broadband Absorption Self-Assembled from Monodispersed Gold Nanospheres by Using a Reverse Emulsion System. , 2015, Angewandte Chemie.

[27]  M. Weeda,et al.  The hydrogen economy – Vision or reality? , 2015 .

[28]  Mohammad Khaja Nazeeruddin,et al.  Water photolysis at 12.3% efficiency via perovskite photovoltaics and Earth-abundant catalysts , 2014, Science.

[29]  Benxia Li,et al.  Metal/Semiconductor Hybrid Nanostructures for Plasmon‐Enhanced Applications , 2014, Advanced materials.

[30]  A. Manivannan,et al.  Solar hydrogen generation by a CdS-Au-TiO2 sandwich nanorod array enhanced with Au nanoparticle as electron relay and plasmonic photosensitizer. , 2014, Journal of the American Chemical Society.

[31]  M. Ouyang,et al.  Controlling Structural Symmetry of a Hybrid Nanostructure and its Effect on Efficient Photocatalytic Hydrogen Evolution , 2014, Advanced materials.

[32]  Shaoming Huang,et al.  Ascorbic-acid-assisted growth of high quality M@ZnO: a growth mechanism and kinetics study. , 2013, Nanoscale.

[33]  Zhenyi Zhang,et al.  Au@TiO2-CdS ternary nanostructures for efficient visible-light-driven hydrogen generation. , 2013, ACS applied materials & interfaces.

[34]  Jianfang Wang,et al.  Fabrication of Au nanotube arrays and their plasmonic properties. , 2013, Nanoscale.

[35]  Martin Moskovits,et al.  An autonomous photosynthetic device in which all charge carriers derive from surface plasmons. , 2013, Nature nanotechnology.

[36]  J. Shapter,et al.  Gold nanotube membranes have catalytic properties , 2012 .

[37]  Thomas Søndergaard,et al.  Plasmonic black gold by adiabatic nanofocusing and absorption of light in ultra-sharp convex grooves , 2012, Nature Communications.

[38]  Franz Faupel,et al.  Design of a Perfect Black Absorber at Visible Frequencies Using Plasmonic Metamaterials , 2011, Advanced materials.

[39]  Claire M. Cobley,et al.  Controlling the synthesis and assembly of silver nanostructures for plasmonic applications. , 2011, Chemical reviews.

[40]  G. Smith,et al.  Hydrogen production from formic acid decomposition at room temperature using a Ag-Pd core-shell nanocatalyst. , 2011, Nature nanotechnology.

[41]  G. Marbán,et al.  Towards the hydrogen economy , 2007 .

[42]  J. Dumesic,et al.  Gold-nanotube membranes for the oxidation of CO at gas-water interfaces. , 2004, Angewandte Chemie.

[43]  M. Jaroniec,et al.  A flexible bio-inspired H2-production photocatalyst , 2018 .

[44]  Lim Wei Yap,et al.  Black Gold: Broadband, High Absorption of Visible Light for Photochemical Systems , 2017 .