Developing efficient homojunctions on g-CN promises metal-free photocatalysis to realize truly sustainable artificial photosynthesis. However, current designs are limited by hindered charge separation due to inevitable grain boundaries and random formation of ineffective homojunctions embedded within the photocatalyst. Here, efficient photocatalysis is driven by introducing effective surface homojunctions on chemically and structurally identical g-CN through leveraging its size-dependent electronic properties.
View Article and Find Full Text PDFIntegrating plasmonic nanoparticles with photonic crystals holds immense potential to enhance green hydrogen photosynthesis by amplifying localized electromagnetic field through generating surface plasmons and slow photons. Current plasmonic photonic designs primarily employ semiconductor-based structural backbone deposited with plasmonic nanoparticles. However, the competition between various optical phenomena in these ensembles hinders effective field enhancement rather than facilitating it.
View Article and Find Full Text PDFEfficient green hydrogen production through electrocatalytic water splitting serves as a powerful catalyst for realizing a carbon-free hydrogen economy. However, current electrocatalytic designs face challenges such as poor hydrogen evolution reaction (HER) performance (Tafel slope, 100-140 mV dec ) because water molecules are thermodynamically trapped within their extensive hydrogen bonding network. Herein, we drive efficient HER by manipulating the local water microenvironment near the electrocatalyst.
View Article and Find Full Text PDFPlasmon-mediated catalysis utilizing hybrid photocatalytic ensembles promises effective light-to-chemical transformation, but current approaches suffer from weak electromagnetic field enhancements from polycrystalline and isotropic plasmonic nanoparticles as well as poor utilization of precious co-catalyst. Here, efficient plasmon-mediated catalysis is achieved by introducing a unique catalyst-on-hotspot nanoarchitecture obtained through the strategic positioning of co-photocatalyst onto plasmonic hotspots to concentrate light energy directly at the point-of-reaction. Using environmental remediation as a proof-of-concept application, the catalyst-on-hotspot design (edge-AgOcta@CuO) enhances photocatalytic advanced oxidation processes to achieve superior organic-pollutant degradation at ≈81% albeit having lesser CuO co-photocatalyst than the fully deposited design (full-AgOcta@CuO).
View Article and Find Full Text PDFPhotothermal steam generation promises decentralized water purification, but current methods suffer from slow water evaporation even at high photothermal efficiency of ≈98%. This drawback arises from the high latent heat of vaporization that is required to overcome the strong and extensive hydrogen bonding network in water for steam generation. Here, light-to-vapor conversion is boosted by incorporating chaotropic/kosmotropic chemistries onto plasmonic nanoheater to manipulate water intermolecular network at the point-of-heating.
View Article and Find Full Text PDFPlasmonic catalysis promises green ammonia synthesis but is limited by the need for co-catalysts and poor performances due to weak electromagnetic field enhancement. Here, we use two-dimensional plasmonic superlattices with dense electromagnetic hotspots to boost ambient nitrogen-to-ammonia photoconversion without needing co-catalyst. By organizing Ag octahedra into a square superlattice to concentrate light, the ammonia formation is enhanced by ≈15-fold and 4-fold over hexagonal superlattice and disorganized array, respectively.
View Article and Find Full Text PDFSpeedy, point-of-need detection and monitoring of small-molecule metabolites are vital across diverse applications ranging from biomedicine to agri-food and environmental surveillance. Nanomaterial-based sensor (nanosensor) platforms are rapidly emerging as excellent candidates for versatile and ultrasensitive detection owing to their highly configurable optical, electrical and electrochemical properties, fast readout, as well as portability and ease of use. To translate nanosensor technologies for real-world applications, key challenges to overcome include ultralow analyte concentration down to ppb or nM levels, complex sample matrices with numerous interfering species, difficulty in differentiating isomers and structural analogues, as well as complex, multidimensional datasets of high sample variability.
View Article and Find Full Text PDFA liquid-liquid interfacial reaction combines reactants with large polarity disparity to achieve greener and more efficient chemistry that is otherwise challenging in traditional single-phase systems. However, current interfacial approaches suffer from the need for a large amount of solvent/reactant/emulsifier and poor reaction performance arising from intrinsic thermodynamic constraints. Herein, we achieve an efficient interfacial reaction by creating a magnetic-responsive, microscale liquid-liquid interface and exploit its dynamic spinning motion to generate vortex-like hydrodynamic flows that rapidly converge biphasic reactants to the point-of-reaction.
View Article and Find Full Text PDFPopulation-wide surveillance of COVID-19 requires tests to be quick and accurate to minimize community transmissions. The detection of breath volatile organic compounds presents a promising option for COVID-19 surveillance but is currently limited by bulky instrumentation and inflexible analysis protocol. Here, we design a hand-held surface-enhanced Raman scattering-based breathalyzer to identify COVID-19 infected individuals in under 5 min, achieving >95% sensitivity and specificity across 501 participants regardless of their displayed symptoms.
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