Angew Chem Int Ed Engl
November 2024
Intramolecular charge separation driving force and linkage chemistry between building blocks are critical factors for enhancing the photocatalytic performance of metal-covalent organic framework (MCOF) based photocatalyst. However, robust achieving both simultaneously has yet to be challenging despite ongoing efforts. Here we develop a fully π-conjugated vinylene-linked multivariate donor-π-acceptor MCOF (D-π-A, termed UJN-1) by integrating benzyl cyanides linker with multiple functional building blocks of electron-rich triphenylamine and electron-deficient copper-cyclic trinuclear units (Cu-CTUs) moieties, featuring with strong intramolecular charge separation driving force, extended conjugation degree of skeleton, and abundant active sites.
View Article and Find Full Text PDFThe empty-space-induced depletion region in photoelectrodes severely exacerbates the recombination of electron-hole pairs, thereby reducing the photoelectrochemical (PEC) analytical performance. Herein, the chemical bond that can suppress the potential barrier and overcome the high energy barrier of out-of-plane Ohmic or Schottky contact is introduced into the PEC sensor to eliminate the depletion region and dramatically promote the separation of electron-hole pairs. Specifically, three-dimensional (3D) hierarchically wheatear-like TiO (HWT) nanostructures featuring a large surface area to absorb incident light are crafted as the substrate.
View Article and Find Full Text PDFDesigning photocatalysts with efficient charge transport and abundant active sites for photocatalytic CO reduction in pure water is considered a potential approach. Herein, a nickel-phthalocyanine containing Ni-N active sites-based conjugated microporous polymer (NiPc-CMP), offering highly dispersed metal active sites, satisfactory CO adsorption capability, and excellent light harvesting properties, is engineered as a photocatalyst. By virtue of the covalently bonded bridge, an atomic-scale interface between the NiPc-CMP/Bi WO Z-scheme heterojunction with strong chemical interactions is obtained.
View Article and Find Full Text PDFIn this study, a CRISPR/Cas12a (LbCpf1)-mediated electrochemiluminescence (ECL) paper-based platform on the basis of a three-dimensional (3D) DNA walker was proposed for the ultrasensitive detection of miRNA-141. Initially, 3D-rGO with a tremendous loading space was modified on the paper working electrode (PWE) to construct an excellent conductive substrate and facilitate the growth of AuPd nanoparticles (NPs). Afterward, the AuPd NPs were introduced as the coreaction emitter medium of the 3D-rGO/PWE to provide convenience for the transformation between SO and SO, amplifying the ECL emission of g-CN nanosheets (NSs).
View Article and Find Full Text PDFExploring novel photoactive materials with high photoelectric conversion efficiency plays a crucial role in enhancing the analytical performance of paper-based photoelectrochemical (PEC) biosensor. SnO, which possesses higher photostability and electron mobility, can be regarded as a promising photoactive material. Herein, paper-based one dimensional (1D) domed SnO nanotubes (NTs) have been developed with the template-consumption strategy.
View Article and Find Full Text PDFA novel photoelectrochemical (PEC) aptasensor was fabricated for DNA detection based on the coupling of cosensitization and peroxidase-like catalytic activity. Specifically, the surfaces of branched-TiO nanorods (B-TiO NRs) were modified with Cd and S to obtain B-TiO NRs/CdS hybrid structures, which were subsequently used as matrices to immobilize hairpin DNA (hDNA) probes. CdTe/TCPP (TCPP = -tetra(4-carboxyphenyl)-porphine) used for signal amplification was labeled on the terminal of the hDNA probe.
View Article and Find Full Text PDFExploring efficient luminophores in the electrochemiluminescence (ECL) system is highly desired to pursue a sensitive ECL sensing platform. Herein, the black phosphorus nanosheets (BP NSs) with excellent ECL properties are investigated and serve as the luminophore with the coreactant of peroxydisulfate (SO) solution. Moreover, owing to the overlapping of emission and absorbance spectra, effective resonance energy transfer (RET) is realized between the BP NSs and the introduced Au nanoparticles.
View Article and Find Full Text PDFEfficient separation of electron-hole pairs is vitally crucial to enhancing the analytical performance of paper-based photoelectrochemical (PEC) bioanalysis. Herein, a simple but effective strategy is developed to modulate the effective separation of photogenerated electrons and holes via introducing a polar charge carriers-created (PCC) electric field induced by a classical perovskite ferroelectric BaTiO (BTO). By inserting it between the n-type WO nanoflakes and p-type CuO (WO nanoflakes/BTO/CuO), the photoelectrode is endowed with a renewable PCC electric field, as a sustaining driving force, to guarantee the realization of directional separation of charge carrier (DSCC) strategy in PEC bioanalysis.
View Article and Find Full Text PDFACS Appl Mater Interfaces
November 2019
A wide-spectrum-responsive paper-based photoelectrochemical (PEC) sensor based on black phosphorus (BP) quantum dots (QDs)-sensitized titanium dioxide (TiO-BP QDs) for prostate-specific antigen (PSA) detection was presented herein. Carbon nanotubes (CNTs) were first coated on paper to form a flexible conductive paper electrode. TiO nanoparticles were then in situ synthesized on the CNTs-modified paper working electrode with direct liquid-phase hydrolysis with normal temperature, shirtsleeve operation, and gentle solution.
View Article and Find Full Text PDFThis work reports a microfluidic paper-based photoelectrochemical (μ-PEC) sensing platform for thrombin (TB) detection with electron-transfer tunneling distance regulation (ETTDR) and aptamer target-triggering nicking enzyme signaling amplification (NESA) dual strategies. Specifically, paper-based TiO nanosheets (PTNs) were prepared with an efficient hydrothermal process, serving as the direct pathway for the charge carriers transfer. When CeO-labeled hairpin DNA 3 (HP3) was closely located at the PTNs, the CeO-PTNs heterostructure was formed, which could great facilitate the photogenerated carries separation of CeO.
View Article and Find Full Text PDFBy controlling target-induced signal quencher release, a label-free and modification-free microfluidic paper based photoelectrochemical analytical device (μ-PAD) for cardiac troponin-I (cTnI) detection was designed for the first time. To achieve it, cellulose paper based single-crystalline three-dimensional aloe like TiO arrays (PSATs) were firstly fabricated as the electron transporting material, providing direct pathways for the charge carriers transfer, and subsequently coupled with CdS to form PSATs/CdS heterojunction for extending the solar spectrum response. Meanwhile, positive charged mesoporous silica nanoparticles (PMSNs) were prepared as the nanocarrier to efficient entrap the Cu which could be regarded as signal quencher due to their reaction with CdS to form CuS.
View Article and Find Full Text PDFRutile titanium dioxide (TiO ) is a promising photocatalyst due to its high thermodynamic stability and few intragrain defects. However, it has not yet achieved photocatalytic activity comparable to that of anatase TiO owing to its higher recombination rate of electron-hole pairs. To effectively separate the electron-hole pairs in rutile TiO , a facet heterojunction (FH) structure to prolong the lifetime of the photogenerated electrons is proposed.
View Article and Find Full Text PDFA bidirectional modulation of photoinduced charge carrier separation strategy based on TiO/BiNbOCl/Co-Pi was proposed in microfluidic paper based photoelectrochemical analytical device (μ-POAD). Perovskite BiNbOCl with high charge carrier mobility was employed as visible light absorber, sandwiching between electron transporting material (ETM) and hole transporting material (HTM). Paper based TiO nanosheet arrays (PTNAs) serve as the ETM to provide a direct pathway for electron transport and Co-Pi works as the HTM to extract holes.
View Article and Find Full Text PDFIn this study, a single-interface photoelectrochemical (PEC) sensor for detecting two antigens, alpha fetoprotein (AFP) and cancer antigen 153 (CA 153), was achieved based on the heterostructure of branched titanium dioxide nanorods (B-TiO NRs)@strontium titanate (SrTiO) heterostructures. The B-TiO NRs@SrTiO heterostructure, prepared by a facile hydrothermal method with the feature of enhanced photogenerated charge carrier separation properties, was first employed as a photoactive substrate for anchored analyst. In order to achieve the goal of successfully detecting two biomarkers at a single interface, the two specific enzyme tags β-galactosidase and acetylcholine esterase linked with a secondary detection antibody were utilized to catalytically hydrolyze p-aminophenyl galactopyranoside and acetylthiocholine to p-aminophenol and thiocholine, respectively.
View Article and Find Full Text PDFThis work described that one-step synthesis three dimensional anatase hierarchically cactus-like TiO arrays (AHCT) and their application in constructing a novel photoelectrochemical (PEC) and visualized sensing platform based on molecular imprinting technique, which reports its result with the prussian blue (PB) electrode served as the electrochromic indicator for the detection of glycoprotein (RNase B). The AHCT arrays were perpendicularly grown on FTO substrate with tunable sizes, offering many advantages, such as large contact area, rapid charge electron separation and transport. A possible formation process of the interesting AHCT arrays has been investigated based on time-dependent experiment.
View Article and Find Full Text PDFBy incorporating the Prussian Blue (PB) electrochromic display as cathode, a solar-driven photoelectrochemical (PEC) cell was constructed through combining sandwich-structured graphite-like carbon nitride (g-CN)-Au-branched-titanium dioxide (B-TiO) nanorods as photoanode for self-powered hydrogen peroxide (HO) sensing, which exhibits both direct photoelectrochemical and electrochromic response. The gold nanoparticles (Au NPs) sandwiched between the B-TiO nanorods and the g-CN layer served as electron relay as well as plasmonic photosensitizer to enhance the solar-to-chemical energy conversion efficiency. Owing to the effective disproportionation of HO and specific recognition of mannose on cell surface, concanavalin-A conjugated porous AuPd alloy nanoparticles were introduced as the catalytically active nanolabels promoting generation of hydroxyl radicals (·OH).
View Article and Find Full Text PDFThe performance of organolead halide perovskites based solar cells has been enhanced dramatically due to the morphology control of the perovskite films. In this paper, we present a fast solvent-assisted molecule inserting (S-AMI) strategy to grow high-quality perovskite film, in which the methylammonium iodide/2-propanol (MAI/IPA) solution is spin-coated onto a dimethylformamide (DMF) wetted mixed lead halide (PbX2) precursor film. The DMF can help the inserting of MAI molecules into the PbX2 precursor film and provide a solvent environment to help the grain growth of the perovskite film.
View Article and Find Full Text PDFA platelike tungsten trioxide (WO3) sensitized with CdS quantum dots (QDs) heterojunction is developed for solar-driven, real-time, and selective photoelectrochemical (PEC) sensing of H2O2 in the living cells. The structure is synthesized by hydrothermally growing platelike WO3 on fluorine doped tin oxide (FTO) and subsequently sensitized with CdS QDs. The as-prepared WO3-CdS QDs heterojunction achieve significant photocurrent enhancement, which is remarkably beneficial for light absorption and charge carrier separation.
View Article and Find Full Text PDFIn this work, a novel sensing platform based on visible light driven biofuel cell (BFC) has been facilely designed for sensitive detection of prostate-specific antigen (PSA) with the photo-response bioanode, realizing the dual route energy conversion of light energy and chemical energy to electricity. The hierarchical branched TiO2 nanorods (B-TiO2 NRs) decorated with CdS quantum dots (QDs) act as the substrate to confine glucose dehydrogenase (GDH) for the visible light driven glucose oxidation at the bioanode. Three dimensional flowers like hierarchical carbon/gold nanoparticles/bilirubin oxidase (3D FCM/AuNPs/BOD) bioconjugate served as biocatalyst for O2 reduction at the biocathode.
View Article and Find Full Text PDFA dual functional analytical device performing both energy conversion and electric energy storage based on biofuel cells to implement self-powered point-of-care testing was developed based on a piece of Ti foil.
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