Latest ArticlesAtomically precise metal nanoclusters (NCs) have been deemed as an emerging class of metal nanomaterials owing to fascinating size-dependent physicochemical properties, discrete energy band structure, and quantum confinement effect, which are distinct from conventional metal nanoparticles (NPs). Nevertheless, metal NCs suffer from photoinduced self-oxidative aggregation accompanied by in-situ transformation to metal NPs, markedly reducing the photosensitization of metal NCs. Herein, maneuvering the generic instability of metal NCs, we perform the charge transport impetus comparison between atomically precise metal NCs and plasmonic metal NPs counterpart obtained from in-situ self-transformation of metal NCs in photoelectrochemical (PEC) water splitting reaction. For conceptual demonstration, we proposed two quintessential heterostructures, which include TNTAs-Au25 heterostructure fabricated by electrostatically depositing glutathione (GSH)-protected Au25(GSH)18 NCs on the TiO2 nanotube arrays (TNTAs) substrate, and TNTAs-Au heterostructure constructed by triggering self-transformation of Au25(GSH)18 NCs to plasmonic Au NPs in TNTAs-Au25 via calcination. The results indicate that photoelectrons produced over Au25 NCs are superior to hot electrons of plasmonic Au NPs in stimulating the interracial charge transport toward solar water oxidation. This is mainly ascribed to the significantly accelerated carrier transport kinetics, prolonged carrier lifespan, and substantial photosensitization effect of Au25 NCs compared with plasmonic Au NPs, resulting in the considerably enhanced PEC water splitting performance of TNTAs-Au25 relative to plasmonic TNTAs-Au counterpart under visible light irradiation. Our work would provide important implications for rationally designing atomically precise metal NCs-based photosystems toward solar energy conversion.
Quantum dots (QDs) based heterojunction is a candidate for the photocatalytic CO2 reduction, owing to the large extinction coefficient and easy modification of band structures. However, the van der Waals interaction causes the large charge resistance and strong recombination centers between QDs and host materials, which makes the poor photocatalytic performance. Herein, a covalent bonded CdSeTe QDs and NH2-UiO-66 heterojunction (NUC-x) is constructed through an acylamino (-CONH-). The results indicate that the acylamino between NH2-UiO-66 and CdSeTe QDs can serve as the transfer channels for the photogenerated charges and stabilize the QDs. The optimized NUC-1200 achieved a CO generation rate of 228.68 µmol/g, which is 13 and 4 times higher than that of NH2-UiO-66 and CdSeTe QDs, respectively. This work provides a new avenue for efficient and stable photocatalysis of QDs.
Over the last 50 years, the explosive adoption of modern agricultural practices has led to an enormous increase in the emission of non-biodegradable and highly biotoxic ions into the hydrosphere. Excess intake of such ions, even essential trace elements such as Cu2+ and F−, can have serious consequences on human health. Therefore, to ensure safe drinking water and regulate wastewater discharge, photoelectrochemical (PEC) online sensors were developed, with advantages such as low energy consumption, inherent miniaturization, simple instrumentation, and fast response. However, there is no publicly available systematic review of the recent advances in PEC ion sensors available in the literature since January 2017. Thus, this review covers the various strategies that have been used to enhance the sensitivity, selectivity, and limit of detection for PEC ion sensors. The photoelectrochemically active materials, conductive substrates, electronic transfer, and performance of various PEC sensors are discussed in detail and divided into sections based on the measurement principle and detected ion species. We conclude this review by highlighting the challenges and potential future avenues of research associated with the development of novel high-performance PEC sensors.
This work demonstrates a two-step method to produce oxide-derived Cu nanowires on Cu mesh surface to offer a monolithic catalyst that outstandingly improves the hydrogen production from reforming formaldehyde and water under ambient conditions. Our results not only reveal that the special oxide-derived nanostructure can significantly improve the formaldehyde reforming performance of Cu, but also display that the hydrogen production has a linear relationship with oxygen pressure. Specially, a maximum of 36 times increment in hydrogen generation rate is observed than that without oxygen during the reaction. Density functional theory calculations show that the formaldehyde molecule is adsorbed on Cu surface only when the adsorbed oxygen is in adjacency, and hydrogen release process is the rate-determining step. This work highlights that the activity of deliberately synthesized catalyst can further be promoted by dynamic chemical modulation of surface states during working.
DNAzyme amplifiers have been extensively explored as a useful sensing platform, but single DNAzyme amplifier is limited in biosensing applications by its low sensitivity. Herein, a cascade DNAzyme amplifier was designed by exploiting concurrent amplification cycle principles of toehold-mediated strand displacement reaction (TSDR) and Zn2+-assisted DNAzyme cycle with lower cost and simpler procedures. Compared with single DNAzyme amplifier, the proposed TSDR-propelled cascade DNAzyme amplifier exhibited higher sensitivity by releasing more DNAzyme through TSDR to cleave substrate strand during the DNAzyme cycle. Base on this, let-7a could be sensitively detected in the range of 5–50 nmol/L with a detection limit of 64 pmol/L. Furthermore, the dual signal amplification strategy of the cascade DNAzyme amplifier exhibited excellent selectivity to distinguish single-base mismatched DNA strands, which has been successfully applied to the determination of let-7a in blood serum, showing high promise in early cancer diagnosis.
The application of metal-organic frameworks (MOFs) nanozymes in biosensing has been extensively investigated, however, till now there is still no report on photoelectrochemical (PEC) sensing based on enzyme memetic properties of MOFs. To further expand the utilization of MOFs nanozymes in biosensing, we developed a label-free homogenous PEC aptasensor for the detection of VEGF165, an important cancer biomarker, based on the DNA-regulated peroxidase-mimetic activity of Fe-MIL-88, a type of MOFs. In this strategy, the peroxidase-mimetic property of MOFs is integrated with the label-free homogeneous PEC sensing approach, and highly sensitive detection of VEGF165 is obtained with a detection limit down to 33 fg/mL, superior or comparable to the previously reported values. Moreover, this approach displays outstanding specificity, and has been successfully used to detect VEGF165 added in diluted serum samples. As far as we know, it is the first example to employ the peroxidase-like activity of MOFs in PEC biosensing, which may find potential application in bioanalysis and early disease diagnosis.
Nitrate (NO3−) is widely found in wastewater, which is harmful to human health and water environmental. Electrochemical reduction can convert NO3− to high value-added ammonia (NH3)/ammonium (NH4+) for pollutant removal and resource recovery. Currently, electrochemical nitrate reduction to produce ammonia (ENRA) is mostly focused on the preparation of high-performance catalysts, while ignoring the prerequisite for industrial application as the stable operation and optimal regulation of the process. Therefore, the review focused on wastewater treatment, based on the mechanism of electrochemical nitrate reduction for ammonia production and reactor construction (reactor, power supply system), then summarized the operation control strategies (such as reduction potential, nitrate concentration, inorganic ions, pH) that should be noted for ENRA. Finally, the challenges (system structure, economy) and prospects (ammonia recovery process, construction of large-scale ENRA system, application of real wastewater) of the field as it moves towards commercialization were discussed. It is hoped that this review will facilitate the scaling up of ENRA in the wastewater treatment field.
Suzuki coupling reactions between symmetrical monomers were conducted in various mesoporous silica nanoreactors grafted with palladium catalysts, enabling the selective formation of [12]cycloparaphenylene precursor with separate yield up to 25% in one-pot reactions, much higher than that in homogeneous reaction. The spatial nanoconfinement of the nanoreactors promotes the macrocyclization while limits the concomitant linear oligomer formation, offering more possibilities for the synthesis of macrocycles from symmetrical monomers in one-pot reaction.
A regiodivergent hydrophosphorylation of enynes with phosphites has been developed using earth-abundant nickel catalyst. The manipulation of regioselectivity can be achieved by regulating the insertion order of alkyne bonds with (RO)2P(O)–Ni–H or R2P(O)O–Ni–H species, respectively. Under the Ni/Xantphos catalysis, 4,1-hydrophosphorylation is selectively obtained while the adding of acid can promote reactions towards 1,2-addition. By employing an additional Pd–H catalysis, 2,1-hydrophosphorylation is also an accessible task in one-pot reaction. Mechanistic studies and analysis have also been performed to interpret the origin of the regioselective regulation. This work highlights the arts in accessing different regioisomers by diverting common elementary reaction steps.
The biocompatibility and biodegradability of peptide self-assembled materials makes them suitable for many biological applications, such as targeted drug delivery, bioimaging, and tracking of therapeutic agents. According to our previous research, self-assembled fluorescent peptide nanoparticles can overcome the intrinsic optical properties of peptides. However, monochromatic fluorescent nanomaterials have many limitations as luminescent agents in biomedical applications. Therefore, combining different fluorescent species into one nanostructure to prepare fluorescent nanoparticles with multiple emission wavelengths has become a very attractive research area in the bioimaging field. In this study, the tetrapeptide Trp-Trp-Trp-Trp (WWWW) was self-assembled into multicolor fluorescent nanoparticles (TPNPs). The results have demonstrated that TPNPs have the blue, green, red and near infrared (NIR) fluorescence emission wavelength. Moreover, TPNPs have shown excellent performance in multicolor bioimaging, biocompatibility, and photostability. The facile preparation and multicolor fluorescence features make TPNPs potentially useful in multiplex bioanalysis and diagnostics.
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