Tunable green syngas generation from CO2 and H2O with sunlight as the only energy input.

The carbon-neutral synthesis of syngas from CO2 and H2O powered by solar energy holds grand promise for solving critical issues such as global warming and the energy crisis. Here we report photochemical reduction of CO2 with H2O into syngas using core/shell Au@Cr2O3 dual cocatalyst-decorated multistacked InGaN/GaN nanowires (NWs) with sunlight as the only energy input. First-principle density functional theory calculations revealed that Au and Cr2O3 are synergetic in deforming the linear CO2 molecule to a bent state with an O-C-O angle of 116.5°, thus significantly reducing the energy barrier of CO2RR compared with that over a single component of Au or Cr2O3. Hydrogen evolution reaction was promoted by the same cocatalyst simultaneously. By combining the cooperative catalytic properties of Au@Cr2O3 with the distinguished optoelectronic virtues of the multistacked InGaN NW semiconductor, the developed photocatalyst demonstrated high syngas activity of 1.08 mol/gcat/h with widely tunable H2/CO ratios between 1.6 and 9.2 under concentrated solar light illumination. Nearly stoichiometric oxygen was evolved from water splitting at a rate of 0.57 mol/gcat/h, and isotopic testing confirmed that syngas originated from CO2RR. The solar-to-syngas energy efficiency approached 0.89% during overall CO2 reduction coupled with water splitting. The work paves a way for carbon-neutral synthesis of syngas with the sole inputs of CO2, H2O, and solar light.

Highly efficient binary copper-iron catalyst for photoelectrochemical carbon dioxide reduction toward methane.

A rational design of an electrocatalyst presents a promising avenue for solar fuels synthesis from carbon dioxide (CO2) fixation but is extremely challenging. Herein, we use density functional theory calculations to study an inexpensive binary copper-iron catalyst for photoelectrochemical CO2 reduction toward methane. The calculations of reaction energetics suggest that Cu and Fe in the binary system can work in synergy to significantly deform the linear configuration of CO2 and reduce the high energy barrier by stabilizing the reaction intermediates, thus spontaneously favoring CO2 activation and conversion for methane synthesis. Experimentally, the designed CuFe catalyst exhibits a high current density of -38.3 mA⋅cm-2 using industry-ready silicon photoelectrodes with an impressive methane Faradaic efficiency of up to 51%, leading to a distinct turnover frequency of 2,176 h-1 under air mass 1.5 global (AM 1.5G) one-sun illumination.

A microfluidic field-effect transistor biosensor with rolled-up indium nitride microtubes.

Field-effect-transistor (FET) biosensors capable of rapidly detecting disease-relevant biomarkers have long been considered as a promising tool for point-of-care (POC) diagnosis. Rolled-up nanotechnology, as a batch fabrication strategy for generating three-dimensional (3D) microtubes, has been demonstrated to possess unique advantages for constructing FET biosensors. In this paper, we report a new approach combining the two fascinating technologies, the FET biosensor and the rolled-up microtube, to develop a microfluidic diagnostic biosensor. We integrated an excellent biosensing III-nitride material-indium nitride (InN)-into a rolled-up microtube and used it as the FET channel. The InN possesses strong, intrinsic, and stable electron accumulation (~1013 cm-2) on its surface, thereby providing a high device sensitivity. Multiple rolled-up InN microtube FET biosensors fabricated on the same substrate were integrated with a microfluidic channel for convenient fluids handling, and shared the same external electrode (inserted into the microchannel outlet) for gating voltage modulation. Using human immunodeficiency virus (HIV) antibody as a model disease marker, we characterized the analytical performance of the developed biosensor and achieved a limit of detection (LOD) of 2.5 pM for serum samples spiked with HIV gp41 antibodies. The rolled-up InN microtube FET biosensor represents a new type of III-nitride-based FET biosensor and holds significant potential for practical POC diagnosis.

Few-Atomic-Layers Iron for Hydrogen Evolution from Water by Photoelectrocatalysis.

The carbon-free production of hydrogen from water splitting holds grand promise for the critical energy and environmental challenges. Herein, few-atomic-layers iron (FeFAL) anchored on GaN nanowire arrays (NWs) is demonstrated as a highly active hydrogen evolution reaction catalyst, attributing to the spatial confinement and the nitrogen-terminated surface of GaN NWs. Based on density functional theory calculations, the hydrogen adsorption on FeFAL:GaN NWs is found to exhibit a significantly low free energy of -0.13 eV, indicative of high activity. Meanwhile, its outstanding optoelectronic properties are realized by the strong electronic coupling between atomic iron layers and GaN(10i0) together with the nearly defect-free GaN NWs. As a result, FeFAL:GaN NWs/n+-p Si exhibits a prominent current density of ∼ -30 mA cm-2 at an overpotential of ∼0.2 V versus reversible hydrogen electrode with a decent onset potential of +0.35 V and 98% Faradaic efficiency in 0.5 mol/L KHCO3 aqueous solution under standard one-sun illumination.

An electrically pumped surface-emitting semiconductor green laser.

Surface-emitting semiconductor lasers have been widely used in data communications, sensing, and recently in Face ID and augmented reality glasses. Here, we report the first achievement of an all-epitaxial, distributed Bragg reflector (DBR)-free electrically injected surface-emitting green laser by exploiting the photonic band edge modes formed in dislocation-free gallium nitride nanocrystal arrays, instead of using conventional DBRs. The device operates at ~523 nm and exhibits a threshold current of ~400 A/cm2, which is over one order of magnitude lower compared to previously reported blue laser diodes. Our studies open a new paradigm for developing low-threshold surface-emitting laser diodes from the ultraviolet to the deep visible (~200 to 600 nm), wherein the device performance is no longer limited by the lack of high-quality DBRs, large lattice mismatch, and substrate availability.

Decoupling Strategy for Enhanced Syngas Generation from Photoelectrochemical CO2 Reduction.

Photoelectrochemical CO2 reduction into syngas (a mixture of CO and H2) provides a promising route to mitigate greenhouse gas emissions and store intermittent solar energy into value-added chemicals. Design of photoelectrode with high energy conversion efficiency and controllable syngas composition is of central importance but remains challenging. Herein, we report a decoupling strategy using dual cocatalysts to tackle the challenge based on joint computational and experimental investigations. Density functional theory calculations indicate the optimization of syngas generation using a combination of fundamentally distinctive catalytic sites. Experimentally, by integrating spatially separated dual cocatalysts of a CO-generating catalyst and a H2-generating catalyst with GaN nanowires on planar Si photocathode, we report a record high applied bias photon-to-current efficiency of 1.88% and controllable syngas products with tunable CO/H2 ratios (0-10) under one-sun illumination. Moreover, unassisted solar CO2 reduction with a solar-to-syngas efficiency of 0.63% is demonstrated in a tandem photoelectrochemical cell.

Photodeposition of a conformal metal oxide nanocoating.

A versatile photochemical route is reported to access conformal metal oxide nanocoatings including Cr2O3, Al2O3, ZnO and In2O3 on semiconductor substrates. The Cr2O3 nanocoating can enhance the photoelectrochemical performance of GaN nanowires on a p-n junction Si photoelectrode, which exhibits a benchmark half-cell solar to hydrogen efficiency of 11.8%.

Structural origin of the high-performance light-emitting InGaN/AlGaN quantum disks.

Ternary III-nitride-based nanowires with highly efficient light-emitting properties are essential for a broad range of applications. By using the selective area molecular-beam epitaxy method, InGaN/AlGaN quantum disks (QDs) embedded in hexagonal GaN nanowires were successfully grown. With the help of atomic-scale-resolved transmission electron microscopy and atom probe tomography, atomic ordering and other related structural information, such as crystallography and local chemistry, have been unambiguously revealed to provide unique insights into the exceptionally strong photoluminescence enhancements. A boomerang-shaped InGaN/AlGaN QD was identified, and atomic-level 1 : 1 periodic chemical ordering within the boomerang shaped AlGaN layers along the c-direction was revealed, confirming the preferential site occupation of Al-atoms. This type of growth provides a strong suppression of the quantum-confined Stark effect and is thus likely a very strong contributor to the exceptional properties. This work therefore enables us to directly establish the key structural elements necessary to understand the exceptionally strong emission exhibited by these materials. Optimization of the configurations of QDs could be an alternative design tool for developing various advanced LED device applications with well-designed structure and desirable optical properties.