Photoelectrochemical (PEC) activation of benzylic C(sp)-H bonds offers a sustainable and eco-friendly approach to synthesizing high-value chemicals. However, achieving high selectivity for desired products remains a significant challenge. In this study, we developed a BiOCl-modified BiVO (BiVO/BiOCl) heterostructure photoanode for the PEC oxidation of benzylic C(sp)-H bonds.
View Article and Find Full Text PDFImproving the water electrolysis efficiency at high current densities is constrained by the structure of available foam and mesh electrodes, which suffer from internal bubble entrapment. Herein, we used laser powder bed fusion-based 3D printing to fabricate Schwarz Diamond (SD) structure nickel electrodes for water electrolysis. After loading with NiMoFeO as the oxygen evolution reaction catalyst and MoNi-MoO as the hydrogen evolution reaction catalyst, the anion exchange membrane water electrolyzer utilizing SD nickel electrodes achieved a current density of 1 A cm at 1.
View Article and Find Full Text PDFHematite is a promising material for photoelectrochemical (PEC) water oxidation, but its photocurrent is limited by bulk charge recombination and poor oxidation kinetics. In this study, we report a high-performance FeO photoanode achieved through gradient surface gallium doping, utilizing a GaO overlayer on FeOOH precursors via atomic layer deposition (ALD) and co-annealing for Ga diffusion. The Ga-doped layer passivates surface states and modifies the band structure, creating a built-in electric field that enhances the charge separation efficiency.
View Article and Find Full Text PDFCuprous oxide (CuO) as an intrinsic p-type semiconductor is promising for solar energy conversion. The major challenge in fabricating CuO lies in achieving both high transparency and high performance in a tandem device. The CuO photocathodes often employ gold as the back contact layer.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Photoelectrochemical (PEC) water splitting represents a promising approach for harnessing solar energy and transforming it into storable hydrogen. However, the complicated 4-electron transfer process of water oxidation reaction imposes kinetic limitations on the overall efficiency. Herein, we proposed a strategy by substituting water oxidation with the oxidation of ethylene glycol (EG), which is a hydrolysis byproduct of polyethylene terephthalate (PET) plastic waste.
View Article and Find Full Text PDFElectrocatalysis holds the key to enhancing the efficiency and cost-effectiveness of water splitting devices, thereby contributing to the advancement of hydrogen as a clean, sustainable energy carrier. This study focuses on the rational design of Ru nanoparticle catalysts supported on TiN (Ru NPs/TiN) for the hydrogen evolution reaction in alkaline conditions. The as designed catalysts exhibit a high mass activity of 20 A mg at an overpotential of 63 mV and long-term stability, surpassing the present benchmarks for commercial electrolyzers.
View Article and Find Full Text PDFAdv Sci (Weinh)
September 2024
The buried interface between the electron transport layer (ETL) and the perovskite layer plays a crucial role in enhancing the power conversion efficiency (PCE) and stability of n-i-p type perovskite solar cells (PSCs). In this study, the interface between the chemical bath deposited (CBD) titanium oxide (TiO) ETL and the perovskite layer using multi-functional potassium trifluoromethyl sulfonate (SK) is modified. Structural and elemental analyses reveal that the trifluoromethyl sulfonate serves as a crosslinker between the TiO and the perovskite layer, thus improving the adhesion of the perovskite to the TiO ETL through strong bonding of the ─CF and ─SO terminal groups.
View Article and Find Full Text PDFSolar fuels offer a promising approach to provide sustainable fuels by harnessing sunlight. Following a decade of advancement, CuO photocathodes are capable of delivering a performance comparable to that of photoelectrodes with established photovoltaic materials. However, considerable bulk charge carrier recombination that is poorly understood still limits further advances in performance.
View Article and Find Full Text PDFCuprous oxide (CuO) is a promising oxide material for photoelectrochemical water splitting (PEC), and increasing its photovoltage is the key to creating efficient overall PEC water-splitting devices. Previous reports are mostly focused on optimizing the energy band alignment between CuO and the n-type buffer layer to improve the photovoltage of CuO photocathodes. However, the band alignment between the n-type buffer layer and the protective layer is often ignored.
View Article and Find Full Text PDFHalide perovskites solar cells are now approaching commercialisation. In this transition from academic research towards industrialisation, standardized testing protocols and reliable dissemination of performance metrics are crucial. In this study, we analyze data from over 16,000 publications in the Perovskite Database to investigate the assumed equality between the integrated external quantum efficiency and the short circuit current from JV measurements.
View Article and Find Full Text PDFWide-bandgap perovskite solar cells (PSCs) have attracted a lot of attention due to their application in tandem solar cells. However, the open-circuit voltage (V ) of wide-bandgap PSCs is dramatically limited by high defect density existing at the interface and bulk of the perovskite film. Here, an anti-solvent optimized adduct to control perovskite crystallization strategy that reduces nonradiative recombination and minimizes V deficit is proposed.
View Article and Find Full Text PDFThe cement industry is one of the largest contributors to global CO emissions, which has been paid more attention to the research on converting the CO released by the cement production process. It is extremely challenging to decarbonize the cement industry, as most CO emissions result from the calcination of limestone (CaCO) into CaO and CO. In this work, we demonstrate an electrochemical process that transforms CaCO into portlandite (Ca(OH), a key Portland cement precursor) and valuable carbonaceous products, which integrates electrochemical water splitting and CO reduction reaction with the chemical decomposition of CaCO.
View Article and Find Full Text PDFAbout 10% efficient antimony selenosulfide (Sb (S,Se) ) solar cell is realized by using selenourea as a hydrothermal raw material to prepare absorber layers. However, tailoring the bandgap of hydrothermal-based Sb (S,Se) film to the ideal bandgap (1.3-1.
View Article and Find Full Text PDFDuring the last decade lead halide perovskites have shown great potential for photovoltaic applications. However, the stability of perovskite solar cells still restricts commercialization, and lack of properly implemented unified stability testing and disseminating standards makes it difficult to compare historical stability data for evaluating promising routes towards better device stability. Here, we propose a single indicator to describe device stability that normalizes the stability results with respect to different environmental stress conditions which enables a direct comparison of different stability results.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2022
Vapor-transport deposition (VTD) method is the main technique for the preparation of SbSe films. However, oxygen is often present in the vacuum tube in such a vacuum deposition process, and SbO is formed on the surface of SbSe because the bonding of Sb-O is formed more easily than that of Sb-Se. In this work, the formation of SbO and thus the carrier transport in the corresponding solar cells were studied by tailoring the deposition microenvironment in the vacuum tube during SbSe film deposition.
View Article and Find Full Text PDFACS Cent Sci
September 2022
Parkinson's disease (PD) is a neurodegenerative disorder characterized by the gradual loss of dopaminergic neurons in the substantia nigra and the accumulation of α-synuclein aggregates called Lewy bodies. Here, nanodecoys were designed from a rabies virus polypeptide with a 29 amino acid (RVG29)-modified red blood cell membrane (RBCm) to encapsulate curcumin nanocrystals (Cur-NCs), which could effectively protect dopaminergic neurons. The RVG29-RBCm/Cur-NCs nanodecoys effectively escaped from reticuloendothelial system (RES) uptake, enabled prolonged blood circulation, and enhanced blood-brain barrier (BBB) crossing after systemic administration.
View Article and Find Full Text PDFThere exists a considerable density of interaggregate grain boundaries (GBs) and intra-aggregate GBs in polycrystalline perovskites. Mitigation of intra-aggregate GBs is equally notable to that of interaggregate GBs as intra-aggregate GBs can also cause detrimental effects on the photovoltaic performances of perovskite solar cells (PSCs). Here, we demonstrate full-scale GB mitigation ranging from nanoscale intra-aggregate to submicron-scale interaggregate GBs, by modulating the crystallization kinetics using a judiciously designed brominated arylamine trimer.
View Article and Find Full Text PDFParkinson's disease (PD) is the second most common neurodegenerative disease globally, and there is currently no effective treatment for this condition. Excessive accumulation of reactive oxygen species (ROS) and neuroinflammation are major contributors to PD pathogenesis. Herein, ultrasmall nanoscale coordination polymers (NCPs) coordinated by ferric ions and natural product curcumin (Cur) were exploited, showing efficient neuroprotection by scavenging excessive radicals and suppressing neuroinflammation.
View Article and Find Full Text PDFACS Appl Mater Interfaces
June 2022
Slow water oxidation kinetics and poor charge transport restrict the development of efficient BiVO photoanodes for photoelectrochemical (PEC) water splitting. Oxygen vacancy as an effective strategy can significantly enhance charge transport and improve conductivity in semiconductor photoanodes. Herein, we obtained BiVO photoanodes with appropriate oxygen vacancy by treating them with hypophosphite, which significantly improved the PEC performance.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
June 2022
The electrochemical nitrate reduction reaction (NITRR) provides a promising solution for restoring the imbalance in the global nitrogen cycle while enabling a sustainable and decentralized route to source ammonia. Here, we demonstrate a novel electrocatalyst for NITRR consisting of Rh clusters and single-atoms dispersed onto Cu nanowires (NWs), which delivers a partial current density of 162 mA cm for NH production and a Faradaic efficiency (FE) of 93 % at -0.2 V vs.
View Article and Find Full Text PDFMitochondrial dysfunction is commonly detected in individuals suffering from Parkinson's disease (PD), presenting within the form of excessive reactive oxygen species (ROS) generation as well as energy metabolism. Overcoming this dysfunction within brain tissues is an effective approach to treat PD, while unluckily, the blood-brain barrier (BBB) substantially impedes intracerebral drug delivery. In an effort to improve the delivery of efficacious therapeutic drugs to the brain, a drug delivery platform hydrogel (MAG-NCs@Gel) was designed by complexing magnolol (MAG)-nanocrystals (MAG-NCs) into the noninvasive thermosensitive poly(-isopropylacrylamide) (PNIPAM) with self-gelation.
View Article and Find Full Text PDFACS Appl Mater Interfaces
November 2021
Cuprous oxide (CuO) is a promising photocathode material for photoelectrochemical (PEC) water splitting. Recently, the PEC performances of CuO-based devices have been considerably improved by introducing nanostructures, semiconductor overlayers, and hydrogen evolution reaction (HER) catalysts. However, CuO devices still suffer from poor stability in aqueous solution, especially in strong acidic or alkaline conditions, despite the use of an intrinsically stable oxide overlayer as a protection layer.
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