Simultaneous Photocatalytic CO Reduction and HO Oxidation Under Non-Sacrificial Ambient Conditions.

The utilization of CO, HO, and solar energy is regarded as a sustainable route for converting CO into chemical feedstocks, paving the way for carbon neutrality and reclamation. However, the simultaneous photocatalytic CO reduction and HO oxidation under non-sacrificial ambient conditions is still a significant challenge. Researchers have carried out extensive exploration and achieved dramatic developments in this area.

Identification of Omitted Pollutants in Environmental Water via In Situ Thin-Film Microextraction.

Sample preparation is an inevitable step in the screening workflow for the identification of unknown pollutants in the aquatic environment. However, the possible loss of pollutants during sample preparation has aroused serious concern but remains not effectively resolved. This study shows that high-risk pollutants omitted in solid-phase extraction (SPE) can be identified via in situ thin-film microextraction (TFME) coupled with high-resolution mass spectrometry.

Achieving a solar-to-chemical efficiency of 3.6% in ambient conditions by inhibiting interlayer charges transport.

Efficiently converting solar energy into chemical energy remains a formidable challenge in artificial photosynthetic systems. To date, rarely has an artificial photosynthetic system operating in the open air surpassed the highest solar-to-biomass conversion efficiency (1%) observed in plants. In this study, we present a three-dimension polymeric photocatalyst achieving a solar-to-HO conversion efficiency of 3.

Construction of Conjugated Organic Polymers for Efficient Photocatalytic Hydrogen Peroxide Generation with Adequate Utilization of Water Oxidation.

The visible-light-driven photocatalytic production of hydrogen peroxide (HO) is currently an emerging approach for transforming solar energy into chemical energy. In general, the photocatalytic process for producing HO includes two pathways: the water oxidation reaction (WOR) and the oxygen reduction reaction (ORR). However, the utilization efficiency of ORR surpasses that of WOR, leading to a discrepancy with the low oxygen levels in natural water and thereby impeding their practical application.

Oxygen-Centered Organic Radicals-Involved Unified Heterogeneous Self-Fenton Process for Stable Mineralization of Micropollutants in Water.

Removing organic micropollutants from water through photocatalysis is hindered by catalyst instability and substantial residuals from incomplete mineralization. Here, a novel water treatment paradigm, the unified heterogeneous self-Fenton process (UHSFP), which achieved an impressive 32% photon utilization efficiency at 470 nm, and a significant 94% mineralization of organic micropollutants-all without the continual addition of oxidants and iron ions is presented. In UHSFP, the active species differs fundamentally from traditional photocatalytic processes.

On-Site Ratiometric Analysis of UO with High Selectivity.

Uranyl ions (UO) are recognized as important indicators for monitoring sudden nuclear accidents. However, the interferences coexisting in the complicated environmental matrices impart serious constraints on the reliability of current on-site monitoring methods. Herein, a novel ratiometric method for the highly sensitive and selective detection of UO is reported based on a [Eu(diaminoterephthalic acid)] (Eu-DATP) metal-organic framework.

Enhancing Photosynthesis Efficiency of Hydrogen Peroxide by Modulating Side Chains to Facilitate Water Oxidation at Low-Energy Barrier Sites.

Hydrogen peroxide (HO) is a crucial oxidant in advanced oxidation processes. In situ, photosynthesis of it in natural water holds the promise of practical application for water remediation. However, current photosynthesis of HO systems primarily relies on oxygen reduction, leading to limited performance in natural water with low dissolved oxygen or anaerobic conditions found in polluted water.

Rapid analysis of dichlorvos via releasing the phosphate core.

Monitoring the residual dichlorvos (O,O-dimethyl-O-2,2-dichlorovinylphosphate, DDVP) in food has received extensive attention owing to its large consumption in agriculture. However, the previous sensing methods are not time-efficient enough due to the long incubation time for enzyme inhibition (tens of minutes to hours) or bottlenecked by the complicated procedures for senor fabrication. Herein, a novel sensing strategy is proposed based on the hydrolysis of DDVP into PO.

Noncovalent Tagging for Identifying Unknown Contaminants of Specific Bioactivity in Environmental Water.

Identifying contaminants of specific bioactivities from complicated environmental matrices remains costly and time-consuming, as it requires us to not only resolve their structures but also determine their bioactivities. Herein, a novel noncovalent tagging method is integrated in mass spectrometry for identifying unknown contaminants that target dopamine (DA) receptors. Via proteolysis of bovine serum albumin, a stereoselective hexapeptide (ACFAVE) is selected for noncovalently tagging the contaminants that possess the stereostructural characteristics of binding to DA receptors.

Metal-Free Photocatalytic CO Reduction to CH and H O under Non-sacrificial Ambient Conditions.

Photocatalytic CO reduction to CH requires photosensitizers and sacrificial agents to provide sufficient electrons and protons through metal-based photocatalysts, and the separation of CH from by-product O has poor applications. Herein, we successfully synthesize a metal-free photocatalyst of a novel electron-acceptor 4,5,9,10-pyrenetetrone (PT), to our best knowledge, this is the first time that metal-free catalyst achieves non-sacrificial photocatalytic CO to CH and easily separable H O . This photocatalyst offers CH product of 10.

Two-Dimensional Conductive Metal-Organic Framework for Small-Molecule Sensing in Aqueous Solution.

Two-dimensional (2D) conductive metal-organic frameworks (cMOFs) have emerged as powerful transducers for electrochemical sensing. However, electrochemical sensing in aqueous solutions remains at a very early stage for 2D cMOFs. Herein, the interfacial capacitances of a 2D cMOF are utilized for electrochemical sensing for the first time.

Novel lanthanide nanoparticle frameworks for highly efficient photoluminescence and hypersensitive detection.

Despite the excellent luminescent properties of lanthanide clusters (LnCs), their suprastructures that inherit their characteristic luminescent properties are scarcely reported. Herein, novel and highly luminescent suprastructures are synthesized a two-step assembly method to incorporate LnCs in covalent organic frameworks (COFs). COFs are pre-synthesized and decorated with rigid anchoring groups on their nanochannel walls, which provide one-dimensional confined spaces for the subsequent assembly of luminescent LnCs.

Hydrogen bond networks in gas-phase complex anions.

Hydrogen bond networks (HBNs) have piqued the interest of the scientific community due to their crucial roles in nature. However, HBNs that are isolated from complicated backgrounds for unraveling their characteristics are still scarce. Herein, we propose that HBNs exist in complex anions formed between α-cyclodextrin (α-CD) and four benzoic acids (RBAs) in the gas phase.

Identifying a selective oligopeptide clamp in the gas phase.

Oligopeptide foldamers are promising as minimalist functional analogues to proteins. Herein, we report a versatile and cost-effective experimental scheme in the gas phase that can facilely identify selective oligopeptides and unambiguously resolve the corresponding folding conformations. Based on this methodology, a stereoselective oligopeptide clamp targeting β-blockers is successfully identified.

High-quality full-color carbon quantum dots synthesized under an unprecedentedly mild condition.

Carbon quantum dots (CQDs) are highly promising to be applied in light-emitting, chemosensing, and other cutting-edge domains. Herein, we successfully fabricate high-quality full-color CQDs under unprecedentedly low temperature and pressure (85°C, 1.88 bar).

Spontaneous exciton dissociation in organic photocatalyst under ambient conditions for highly efficient synthesis of hydrogen peroxide.

SignificanceHydrogen peroxide is a highly competitive ready-to-use product for solar energy transformation. Nevertheless, the contemporary photosynthetic systems are not efficient enough, due to severe charge recombination caused by high activation energy and binding energy of the exciton. Herein, we achieve spontaneous exciton dissociation at room temperature.

Superficially capped amino metal-organic framework for efficient solid-phase microextraction of perfluorinated alkyl substances.

Perfluorinated alkyl substances (PFASs) were ubiquitously in the surface and groundwater. It is crucial and urgent to develop a rapid and ultrasensitive analysis method for the quantification of trace-level PFASs. Herein, a highly hydrophobic sorbent by capping phenylsilane groups on the surfaces of NH-UiO-66(Zr) nanocrystals was used for efficient solid-phase microextraction (SPME) of PFASs in water samples.

A solar-to-chemical conversion efficiency up to 0.26% achieved in ambient conditions.

Artificial photosynthesis in ambient conditions is much less efficient than the solar-to-biomass conversion (SBC) processes in nature. Here, we successfully mimic the NADP-mediated photosynthetic processes in green plants by introducing redox moieties as the electron acceptors in the present conjugated polymeric photocatalyst. The current artificial process substantially promotes the charge carrier separation efficiency and the oxygen reduction efficiency, achieving a photosynthesis rate for converting Earth-abundant water and oxygen in air into hydrogen peroxide as high as 909 μmol⋅g⋅h and a solar-to-chemical conversion (SCC) efficiency up to 0.

Noncovalently Tagged Gas Phase Complex Ions for Screening Unknown Contaminant Metabolites in Plants.

Screening the metabolites of emerging organic contaminants (EOCs) from complicated biological matrices is an important but challenging task. Although stable isotope labeling (SIL) is frequently used to facilitate the identification of contaminant metabolites from redundant interfering components, the isotopically labeled reagents are expensive and difficult to synthesize, which greatly constrains the application of the SIL method. Herein, a new online noncovalent tagging method was developed for screening the metabolites of 1H-benzotriazol (BT) based on the characteristic structural moieties reserved in the metabolites.

Ratiometric fluorescent probe for the on-site monitoring of coexisted Hg and F in sequence.

The monitoring of mercury and fluoride ions (Hg and F) has aroused wide concerns owing to the high toxicity of Hg and the duplicitous nature of F to human health. As far as we known, more than 100 million people in poverty-stricken areas are still at high risk of being over-exposed to Hg and F via drinking water. Simple and cost-effective luminescent methods are highly promising for on-site water monitoring in rural areas.

Polymer Ligand-Sensitized Lanthanide Metal-Organic Frameworks for an On-Site Analysis of a Radionuclide.

Herein, a new strategy to increase the sensitivity of a lanthanide metal-organic framework (Ln-MOF) to UO was proposed by using polymeric ligands. By utilizing [Tb(1,3,5-benzenetrisbenzoate)]n (Tb-TBT) MOF as the host, preloaded 2-vinyl terephthalic acid (VTP) was polymerized in situ, which produced a novel fluorescent composite denoted as PVTP⊂Tb-TBT. Benefiting from the coordination of PVTP to the Tb nodes, the polymeric chains performed both as molecular scaffolds that improved the water stability of the framework and as additional antennae that sensitized the photoluminescence of the Tb nodes.

Highly efficient photosynthesis of hydrogen peroxide in ambient conditions.

Photosynthesis of hydrogen peroxide (HO) in ambient conditions remains neither cost effective nor environmentally friendly enough because of the rapid charge recombination. Here, a photocatalytic rate of as high as 114 μmol⋅g⋅h for the production of HO in pure water and open air is achieved by using a Z-scheme heterojunction, which outperforms almost all reported photocatalysts under the same conditions. An extensive study at the atomic level demonstrates that Z-scheme electron transfer is realized by improving the photoresponse of the oxidation semiconductor under visible light, when the difference between the Fermi levels of the two constituent semiconductors is not sufficiently large.

Headspace solid-phase microextraction of semi-volatile ultraviolet filters based on a superhydrophobic metal-organic framework stable in high-temperature steam.

Headspace solid-phase microextraction (HS-SPME) of low volatile analytes from complex aqueous samples can be substantially facilitated by elevating the temperature of the samples. However, many SPME coatings prepared from novel sorptive materials may suffer from low stabilities in hot water steam. Herein, a superhydrophobic metal-organic framework (MOF) derived from decorating the metal-oxo nodes of the amino-functionalized UiO-66(Zr) with phenylsilane was prepared and successfully developed into a novel SPME fiber coating.

Valence-dependent catalytic activities of iron terpyridine complexes for pollutant degradation.

Herein, iron-terpyridine complexes with the iron centers at different initial valence states were utilized as homogeneous catalysts for the degradation of phenol in water. The iron(iii)-terpyridine complex induced the formation of more high-valent iron-oxo centers and hydroxyl radicals than the iron(ii)-terpyridine complex, leading to a higher catalytic activity.

Ultrasonic semi-solid coating soldering 6061 aluminum alloys with Sn-Pb-Zn alloys.

In this paper, 6061 aluminum alloys were soldered without a flux by the ultrasonic semi-solid coating soldering at a low temperature. According to the analyses, it could be obtained that the following results. The effect of ultrasound on the coating which promoted processes of metallurgical reaction between the components of the solder and 6061 aluminum alloys due to the thermal effect.