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Limited charge separation/transport efficiency remains the primary obstacle of achieving satisfying photoelectrochemical (PEC) water splitting performance. Therefore, it is essential to develop diverse interfacial engineering strategies to mitigate charge recombination. Despite obvious progress having been made, most works only considered a single‐side modulation in either the electrons of conduction band or the holes of valence band in a semiconductor photoanode, leading to a limited PEC performance enhancement. Beyond this conventional thinking, we developed a novel coupling modification strategy to achieve a composite electrode with bidirectional carrier transport for a better charge separation, in which Ti2C3Tx MXene quantum dots (MQDs) and α‐Fe2O3 nanodots (FO) are anchored on the surface of ZnIn2S4 (ZIS) nanoplates, resulting in markedly improved PEC water splitting of pure ZIS photoanode. Systematic studies indicated that the bidirectional charge transfer pathways were stimulated due to MQDs as "electron extractor" and S−O bonds as carriers transport channels, which synergistically favors significantly enhanced charge separation. The enhanced kinetic behavior at the FO/MQDs/ZIS interfaces was systematically and quantitatively evaluated by a series of methods, especially scanning photoelectrochemical microscopy. This work may deepen our understanding of interfacial charge separation, and provide valuable guidance for the rational design and fabrication of high‐performance composite electrodes. [ABSTRACT FROM AUTHOR]

Limited charge separation/transport efficiency remains the primary obstacle of achieving satisfying photoelectrochemical (PEC) water splitting performance. Therefore, it is essential to develop diverse interfacial engineering strategies to mitigate charge recombination. Despite obvious progress having been made, most works only considered a single‐side modulation in either the electrons of conduction band or the holes of valence band in a semiconductor photoanode, leading to a limited PEC performance enhancement. Beyond this conventional thinking, we developed a novel coupling modification strategy to achieve a composite electrode with bidirectional carrier transport for a better charge separation, in which Ti2C3Tx MXene quantum dots (MQDs) and α‐Fe2O3 nanodots (FO) are anchored on the surface of ZnIn2S4 (ZIS) nanoplates, resulting in markedly improved PEC water splitting of pure ZIS photoanode. Systematic studies indicated that the bidirectional charge transfer pathways were stimulated due to MQDs as "electron extractor" and S−O bonds as carriers transport channels, which synergistically favors significantly enhanced charge separation. The enhanced kinetic behavior at the FO/MQDs/ZIS interfaces was systematically and quantitatively evaluated by a series of methods, especially scanning photoelectrochemical microscopy. This work may deepen our understanding of interfacial charge separation, and provide valuable guidance for the rational design and fabrication of high‐performance composite electrodes. [ABSTRACT FROM AUTHOR]

In privacy protection methods based on location services, constructing anonymous areas using location information shared by collaborative users is the main method. However, this collaborative process not only increases the risk of mobile users' location privacy being leaked, but also reduces positioning accuracy. In response to this problem, we propose a balancing strategy, which transforms the problem of protecting mobile users' location privacy and improving positioning accuracy into a balance issue between location privacy and positioning accuracy. The cooperation of mobile users with different collaborating users is then modeled as an objective optimization problem, and location privacy and positioning accuracy are evaluated separately to make different selection strategies. Finally, an optimization function is constructed to select the optimal selection strategies. Experimental results show that our proposed strategy can effectively achieve the balance between location privacy and positioning accuracy. [ABSTRACT FROM AUTHOR]

Depositing a transition‐metal hydroxide (TMH) layer on a photoanode has been demonstrated to enhance photoelectrochemical (PEC) water oxidation. However, the controversial understanding for the improvement origin remains a key challenge to unlock the PEC performance. Herein, by taking BiVO4/iron‐nickel hydroxide (BVO/FxN4−x‐H) as a prototype, we decoupled the PEC process into two processes including charge transfer and surface catalytic reaction. The kinetic information at the BVO/FxN4−x‐H and FxN4−x‐H/electrolyte interfaces was systematically evaluated by employing scanning photoelectrochemical microscopy (SPECM), intensity modulated photocurrent spectroscopy (IMPS) and oxygen evolution reaction (OER) model. It was found that FxN4−x‐H acts as a charge transporter rather than a sole electrocatalyst. PEC performance improvement is mainly ascribed to the efficient suppression of charge recombination by fast hole transfer kinetics at BVO/FxN4−x‐H interface. [ABSTRACT FROM AUTHOR]

Depositing a transition‐metal hydroxide (TMH) layer on a photoanode has been demonstrated to enhance photoelectrochemical (PEC) water oxidation. However, the controversial understanding for the improvement origin remains a key challenge to unlock the PEC performance. Herein, by taking BiVO4/iron‐nickel hydroxide (BVO/FxN4−x‐H) as a prototype, we decoupled the PEC process into two processes including charge transfer and surface catalytic reaction. The kinetic information at the BVO/FxN4−x‐H and FxN4−x‐H/electrolyte interfaces was systematically evaluated by employing scanning photoelectrochemical microscopy (SPECM), intensity modulated photocurrent spectroscopy (IMPS) and oxygen evolution reaction (OER) model. It was found that FxN4−x‐H acts as a charge transporter rather than a sole electrocatalyst. PEC performance improvement is mainly ascribed to the efficient suppression of charge recombination by fast hole transfer kinetics at BVO/FxN4−x‐H interface. [ABSTRACT FROM AUTHOR]

Depositing a transition‐metal hydroxide (TMH) layer on a photoanode has been demonstrated to enhance photoelectrochemical (PEC) water oxidation. However, the controversial understanding for the improvement origin remains a key challenge to unlock the PEC performance. Herein, by taking BiVO4/iron‐nickel hydroxide (BVO/FxN4−x‐H) as a prototype, we decoupled the PEC process into two processes including charge transfer and surface catalytic reaction. The kinetic information at the BVO/FxN4−x‐H and FxN4−x‐H/electrolyte interfaces was systematically evaluated by employing scanning photoelectrochemical microscopy (SPECM), intensity modulated photocurrent spectroscopy (IMPS) and oxygen evolution reaction (OER) model. It was found that FxN4−x‐H acts as a charge transporter rather than a sole electrocatalyst. PEC performance improvement is mainly ascribed to the efficient suppression of charge recombination by fast hole transfer kinetics at BVO/FxN4−x‐H interface. [ABSTRACT FROM AUTHOR]

An effective ratiometric fluorescent probe based on silicon particles/gold nanoclusters (SiNPs/AuNCs) nanohybrid has been fabricated and applied to be a "on-off-on" switch sensing platform for detection of Hg2+ and cysteine. In this elaborated sensing platform, the SiNPs just acted as internal reference signal, providing a build-in correction for background interferences and environmental effects, to which the AuNCs as a signal report unit for Hg2+ response was covalently grafted by amidation reaction. The fluorescence intensity of SiNPs/AuNCs could be effectively quenched upon adding Hg2+, accompanied with an easily distinguishable fluorescent color change. The ratiometric fluorescence signal (F 649 /F 511) of the established nanoprobe was linearly proportional to the concentration of Hg2+ ranging from 0.02 to 24 μM with a low detection limit of 5.6 nM, which is below the guideline value of Hg2+ in drinking water set by the World Health Organization. Interestingly, upon addition of cysteine, the Hg2+-quenched fluorescence intensity was recovered gradually. Furthermore, the approach developed has also been utilized for Hg2+ detection in real complex biological samples with satisfactory results. More importantly, benefiting from the good water-solubility and excellent biocompatibility, this nanoprobe can monitor the intracellular Hg2+ and cysteine in living cells, indicating its potential applications in advanced biosensing and bioimaging. Herein, we reported an effective dual-emission ratiometric probe for "on-off-on" detection of Hg2+ and cysteine. Image 1 • An efficient dual-emission fluorescent probe for simultaneously and visual detecting Hg2+ and L-Cys was constructed. • The probe could simultaneously detection of Hg2+ in human serum and urine samples. • Due to the ratiometric fluorescence model, the background interference was extincted. • The developed probe was successfully used for the fluorescence bioimaging of Hg2+ and L-Cys in live cells. [ABSTRACT FROM AUTHOR]

[Display omitted] • A dual-signal readout sensor with good sensitivity and selectivity has been developed for dopamine detection. • The study of catechol oxidase mimicking MOF nanozymes has the potential to expand the range of biomimetic MOFs. • The type of modular used in the synthesis process of MOFs can influence the activity of the final enzyme. Enzyme-simulating nanomaterials, with obvious advantages of high activity, stability and cost-effectiveness, can surrogate the complex natural enzymes and catalyze enzyme-like reactions in various harsh applications. Herein, a novel fluorescent and colorimetric dual-readout sensing platform toward dopamine detection based on pyrazolate-based porphyrinic metal-organic frameworks (MOFs) by coordination regulation strategy to improve the performance of catechol oxidase mimic enzyme activity was constructed. Specifically, BA (benzoic acid) or PA (4-Formyl-1(H)-pyrazole) was introduced as auxiliary ligands to regulate the growth mode of pyrazolate-based porphyrinic MOF materials. H 4 TPP (5,10,15,20-Tetra(1 H -pyrazol-4-yl) porphyrin) and auxiliary ligands coordinated with Cu(II), exposing Cu sites with insufficient coordination and enhancing the interaction with oxygen-active species. Benefiting from the binuclear copper center structure and the preferential adsorption of reactants in the self-reinforced interface, a highly sensitive and selective detection method for dopamine based on Cu-TPP(PA) MOF material was proposed under the intervention of H 2 O 2. The feasibility of Cu-TPP(PA) MOF in detecting dopamine in human serum samples and as a paper-based analytical device was investigated. This achievement will expand the applications of MOFs in analytical chemistry and open up a new avenue for the design of highly active and stable nano-enzymes. [ABSTRACT FROM AUTHOR]

Solar-driven CO 2 reduction into valuable liquid fuels with H 2 O oxidation presents a very promising approach for sustainable carbon cycle to achieve carbon neutral. The PdIn@N 3 -COF exhibits a record-high total yield of alcohols of 798 μmol g−1 (CH 3 OH 74 %, and CH 3 CH 2 OH 26 %) among the COF and MOF materials as the synergy in both the bimetallic nanocluster and cluster-framework. • Solar-driven CO 2 reduction into valuable liquid fuels with H 2 O oxidation. • A facile strategy for filling bimetallic PdIn nanoclusters into covalent organic framework. • Record-high total yield for conversion of CO 2 -to-alcohols among the framework materials. • Unique synergistic effect for conversion of CO 2 to C 2 alcohols. Solar-driven CO 2 reduction with H 2 O oxidation into liquid fuels is highly desirable for sustainable carbon cycle to achieve carbon neutral, but represents a great challenge for artificial photosynthesis. Herein, bimetallic PdIn nanoclusters are confined in a photosensitizing covalent organic framework (N 3 -COF) to facilely construct Pd x In y @N 3 -COF composites (x:y = 1:0, 0:1, 1:2, 1:1, 2:1). The resulting PdIn@N 3 -COF exhibits excellent activity for CO 2 photoreduction with H 2 O oxidation as the H+ and e− source, showing a record-high total yield of 798 μmol g-1 for producing CH 3 OH (74 %) and CH 3 CH 2 OH (26 %) among the framework materials. The synergy in both the bimetallic nanocluster and cluster@N 3 -COF contributes greatly to C C coupling and interfacial charge transfer, thus achieving excellent activity for conversion of CO 2 to C 1 /C 2 alcohols on the non-copper catalysts. This work highlights the amazing potential for constructing bimetallic nanocluster@photosensitizing supports to produce alcohols in artificial photosynthesis with H 2 O oxidation. [ABSTRACT FROM AUTHOR]

[Display omitted] Photocatalysis utilizing solar energy is a promising strategy for mitigating energy crisis and environmental pollution. Exploring a cost-effective, stable, eco-friendly, and efficient photocatalytic system is extremely urgent. Herein, copper encapsulated within nitrogen-doped carbon nanosphere (Cu@N C) possessing a unique core-shell structure with high catalytic activity was prepared by ion-exchange and pyrolysis using resin as support. The protective carbon shell can prevent the leaching of metal ions and deactivation of the catalyst. Benefiting from the special structure, Cu@N C exhibited excellent activity and durability toward the degradation of tetracycline by the activation of peroxymonosulfate (PMS). The radical trapping experiments and electron spin resonance analyses were applied to elucidate the main reactive species. This work highlights the great potential of Cu@N C core-shell nanosphere as photocatalyst, which provides a new opportunity for the remediation of environmental pollution. [ABSTRACT FROM AUTHOR]

Gold clusters loaded on various supports have been widely used in the fields of energy and biology. However, the poor photostability of Au clusters on support interfaces under prolonged illumination usually results in loss of catalytic performance. Covalent organic frameworks (COFs) with periodic and ultrasmall pore structures are ideal supports for dispersing and stabilizing Au clusters, although it is difficult to encapsulate Au clusters in the ultrasmall pores. In this study, a two‐dimensional (2D) COF modified with thiol chains in its pores was prepared. With −SH groups as nucleation sites, Au nanoclusters (NCs) could grow in situ within the COF. The ultrasmall pores of the COF and the strong S−Au binding energy combine to improve the dispersibility of Au NCs under prolonged light illumination. Interestingly, Au–S–COF bridging as observed in this artificial Z‐scheme photocatalytic system is deemed to be an ideal means to increase charge‐separation efficiency. [ABSTRACT FROM AUTHOR]

Gold clusters loaded on various supports have been widely used in the fields of energy and biology. However, the poor photostability of Au clusters on support interfaces under prolonged illumination usually results in loss of catalytic performance. Covalent organic frameworks (COFs) with periodic and ultrasmall pore structures are ideal supports for dispersing and stabilizing Au clusters, although it is difficult to encapsulate Au clusters in the ultrasmall pores. In this study, a two‐dimensional (2D) COF modified with thiol chains in its pores was prepared. With −SH groups as nucleation sites, Au nanoclusters (NCs) could grow in situ within the COF. The ultrasmall pores of the COF and the strong S−Au binding energy combine to improve the dispersibility of Au NCs under prolonged light illumination. Interestingly, Au–S–COF bridging as observed in this artificial Z‐scheme photocatalytic system is deemed to be an ideal means to increase charge‐separation efficiency. [ABSTRACT FROM AUTHOR]

Porphyrins, as significant electrochemical luminaries, have garnered extensive attention due to their distinctive structure and superior photoelectric properties in recent years. However, the potential aggregation resulting from water insolubility in aqueous phases, as well as its inherent instability and weaker Q-band, continue to pose challenges for the electrochemiluminescence (ECL) applications of porphyrins. This review provides a comprehensive summary of different strategies aimed at achieving high efficiency of porphyrin in ECL and signal amplification. Finally, a critical perspective and future prospects regarding the developmental trends of porphyrins are presented. • Porphyrin-based luminophores were summarized. • Auxiliary strategies for signal amplification were discussed. • A critical perspective and future prospects regarding the developmental trends of porphyrins was presented. [ABSTRACT FROM AUTHOR]

BV/In 2 O 3 /FeNi photoanode was rational designed and constructed by impregnation annealing and electrodeposition method. A stable photocurrent of 4.0 mA cm−2 was achieved at 1.23 V RHE under AM 1.5 G (100 mW cm−2), which can be ascribed to the synergistic effect of heterojunction structure and cocatalyst loading. [Display omitted] Bismuth vanadate (BiVO 4) is a promising nanomaterial for photoelectrochemical (PEC) water oxidation. However, the serious charge recombination and sluggish water oxidation kinetics limit its performance. Herein, an integrated photoanode was successfully constructed by modifying BiVO 4 (BV) with In 2 O 3 (In) layer and further decorating amorphous FeNi hydroxides (FeNi). The BV/In/FeNi photoanode exhibited a remarkable photocurrent density of 4.0 mA cm−2 at 1.23 V RHE , which is approximately 3.6 times larger than that of pure BV. And the water oxidation reaction kinetics has an over 200% increased. This improvement was mainly because the formation of BV/In heterojunction inhibited charge recombination, and the decoration of cocatalyst FeNi facilitated the water oxidation reaction kinetics and accelerated hole transfer to electrolyte. Our work provides another possible route to develop high-efficiency photoanodes for practical applications in solar conversion. [ABSTRACT FROM AUTHOR]

The electrochemical nitrogen reduction reaction (NRR) has the potential to replace the Haber–Bosch process for ammonia synthesis under ambient conditions. However, the selectivity and yield of the NRR are impractical, owing to the preferential binding of the electrocatalyst to H and the consequential coverage of active sites. In this study, VO2, with N2 strongly adsorbed over H atoms, is used as a support to provide a N2 source to avoid the hydrogen evolution reaction. Mo, with a high NRR activity, is introduced as the active site to promote the NRR. Meanwhile, the electronic metal–support interaction between the support and Mo creates electron‐deficient sites, which weakens H adsorption and lowers the energy barrier of the first step, protonation, thereby kinetically enhancing the NRR activity. The average NH3 yield of Mo/VO2 is 190.1 µgNH3 mgcat.−1 h−1 and the Faradaic efficiency is 32.4% at −0.5 V versus reversible hydrogen electrode, which is 10.8 and 2.8 times greater than that of VO2, respectively. [ABSTRACT FROM AUTHOR]

Background: Bacterial contamination may cause loss of or damage to cultured oocytes or embryos, resulting in the lack of transplantable embryos during IVF embryo culture. However, there are few reports about IVF embryo contamination caused by embryology laboratories. In this work, we evaluated clinical pregnancy outcomes and the risk of maternal and infant complications after embryo contamination caused by environmental pollution during IVF. Methods: The authors retrospectively analyzed 2490 IVF-ET ovulation induction therapy cycles in the Reproductive Center of Yichang Central People's Hospital from January 2015 to May 2022. According to the presence or absence of embryo culture medium contamination, the two groups were divided into an embryo contamination cycle and a nonembryo contamination cycle. The primary outcome parameters were the characteristics and progress of embryo culture medium contamination. Embryo laboratory outcomes, pregnancy outcomes, and maternal and infant complications were secondary outcome parameters. Results: One case of embryo contamination originated from semen contamination. The remaining 15 cases involved environmental contamination outbreaks in embryo culture chambers, caused by Staphylococcus pasteuri. Compared with conventional uncontaminated IVF cycles, the 15 cases of contaminated embryo cycles showed no significant difference in embryo laboratory outcomes, pregnancy outcomes, or maternal and infant complications except for a slightly higher rate of fetal growth retardation. Ultimately, 11 live-born infants were successfully delivered, of which 2 were premature. The remaining 4 patients did not become pregnant after 1–2 transfers due to a lack of transferable embryos. Conclusion: When the embryo culture medium is contaminated due to the environmental contamination of the IVF culture room, it is feasible to perform daily rapid rinsing of the culture medium and avoid blastocyst culture as remedial treatment. However, the long-term impact on offspring needs further prospective research. [ABSTRACT FROM AUTHOR]

Excessive residues of tetracycline antibiotics (TCs) are very harmful to the ecosystems and human health, thus it is urgent to establish an effective method for both detection and removal of TCs. Herein, the blue luminescent carbon dots (CDs) were synthesized and modified into a hierarchical mesoporous zeolitic imidazolate framework-8 (HZIF-8) which prepared using hydrogel as template to form CDs@HZIF-8 complex. The blue fluorescence of CDs@HZIF-8 at 440 nm was quenched by TCs through internal filtering effect (IFE), meanwhile, the interaction between TCs and Zn2+ led to a significant conformational change of TCs, which enhanced the fluorescence at 536 nm. Based on the reverse change of two fluorescence signals (F 536 / F 440), a ratiometric fluorescence sensor was constructed for the detection of TCs. It is worth mentioning that, thanks to the hierarchical porous structure of CDs@HZIF-8, sufficient space is provided for TCs enrichment in the pores and full contact with the skeleton, which improves the adsorption capacity of TCs and significantly enhances the sensitivity of TCs detection. The detection limits of tetracycline (TC), oxytetracycline (OTC) and doxycycline (DOX) were 6.56 nM, 29.46 nM, and 30.58 nM, respectively. Additionally, the rational design method was successfully applied to detect TCs in milk samples. Herein, CDs@HZIF-8 complex was synthesized for simultaneous ratiometric fluorescence detection and removal of tetracycline antibiotics. [Display omitted] • CDs@HZIF-8 was synthesized and used as a self-calibrating probe for the detection of tetracycline antibiotics. • The detection limits of tetracycline, oxytetracycline and doxycycline were 6.56 nM, 29.46 nM, and 30.58 nM, respectively. • The rational design method was successfully applied to detect tetracycline antibiotics in milk samples. [ABSTRACT FROM AUTHOR]

[Display omitted] • A smart strategy, interface "repairing", was proposed to effectively boost the photogenerated charge separation. • BV/NiO x /CoFe achieves a remarkably photocurrent density of 4.58 mA cm−2 at 1.23 V RHE , which is more than three-fold higher than BV photoanode. • The interface charge recombination and intrinsic photocorrosion can be efficiently suppressed through "fast" hole transfer kinetics. Photoelectrochemical (PEC) water splitting is an attractive strategy to convert and store of intermittent solar power into fuel energy. However, the detrimental charge recombination of photogenerated electrons and holes severely limits its efficiency. Despite electrocatalyst loading can obviously improve the PEC conversion efficiency, current systems still suffer from high recombination owing to the surface states. Herein, an interface "repairing" strategy is proposed to suppress the recombination at the semiconductor/electrocatalyst interface. NiO x layer acts as an interfacial repairing layer to efficiently extract photogenerated charge carriers and eliminate the surface states via high hole-transfer kinetics rather than as a traditional electrocatalyst. As expected, the resulting repaired system yields an impressive photocurrent density of 4.58 mA cm−2 at 1.23 V (vs. RHE), corresponding to a more than three-fold increase compared to BiVO 4 (1.40 mA cm−2). Our work offers an appealing maneuver to improve the water oxidation performance for the semiconductor/electrocatalyst coupling system. [ABSTRACT FROM AUTHOR]

As biologically active small molecular, biogenic amines (BAs) could be served as an important index of food spoilage and contamination. In addition, excessive intake of biogenic amines usually can cause a serious impact on human health. Therefore, it is of great significance to establish a reliable, sensitive, and non-invasive method for the detection of biogenic amines in foods. To address the above problems, optical sensing method utilizing dual-channel fluorescence outputs could be considered as a powerful technique, which can achieve high accuracy and even visual detection. Herein, we have demonstrated for the first time the use of a dual-channel luminescent signal readout nanoprobe o -CDs@methyl red (CDs stands for carbon dots) for rapid, sensitive, and visual detection of biogenic amines. Such probe was prepared by covalently modifying methyl red on NH 2 -rich carbon dots, in which o -CDs served as a reference signal and methyl red acted as a signal report unit for BAs. Upon the addition of BAs, the fluorescence intensity of methyl red increases, while that of o -CDs remains almost unchanged. It was found that such fluorescence platform can detect tyramine with high sensitivity (LOD: 0.01 μ M) and fast response (30 s). More importantly, the proposed method can be successfully applied for biogenic amines detection in real milk and yogurt samples, indicating that the as-prepared probe holds the further potential for practical application in control and monitoring of food quality and freshness. [Display omitted] Herein, we reported a dual-signal fluorescent sensing platform for biogenic amine detection in milk and yogurt. • A dual-signal fluorescent sensing platform based on o -CDs@methyl red was synthesized. • Dual-channel luminescent sensor greatly improves the reliability of the detection result. • The developed probe is able to analyze tyramine with a low detection limit of 0.01 μ M. • The proposed method was successfully applied for determination the trace amount of biogenic amines in milk and yogurt samples. [ABSTRACT FROM AUTHOR]

Taking porphyrin and polyaniline as hole transfer layers simultaneously between BV and OEC, a novel multi-step hole transfer strategy was proposed to enhance PEC water splitting. The constructed system can effectively accelerate hole transport kinetics and suppress the interface recombination of charge carriers, resulting in a high PEC performance. [Display omitted] • A novel strategy was proposed to accelerate hole transport and suppress interface recombination. • BV/CoPy/PANI/CoFe photoanode exhibited excellent water oxidation capability. • The photocurrent of BV/CoPy/PANI/CoFe is 4.5 mA cm−2 at 1.23 V RHE under AM 1.5 G illumination. • IMPS and SPECM measurements revealed the mechanism of charge transfer kinetics. • This work provides an effective guideline for designing excellent photoanodes. Serious surface recombination and sluggish reaction kinetics hamper the photoelectrochemical (PEC) performance from being efficient. Although coupling oxygen evolution catalysts on photoanodes to accelerate electrode reactions has been demonstrated an effective strategy to enhance photocurrent, the surface recombination still limits the performance to an ideal level. Herein, a novel multi-step hole transfer strategy is developed for accelerating hole transport and thus suppressing the surface recombination. In this system, porphyrin and polyaniline both act as hole transfer layers, which construct an effective stair-stepping hole transfer channel to ensure much more holes take part in water oxidation process. This simple interface modulation system exhibits a remarkable photocurrent of 4.5 mA cm−2 at 1.23 V (vs. reversible hydrogen electrode (RHE), AM 1.5 G illumination) accompanied with good stability and provides a promising strategy for the design of efficient photoanodes for solar conversion. [ABSTRACT FROM AUTHOR]

Coating photoanodes with transition‐metal hydroxides (TMH) is a promising approach for improving photoelectrochemical (PEC) water oxidation. However, the present system still suffers from high charge recombination and sluggish surface reactions. Herein, effective charge separation is achieved at the same time as boosting the surface catalytic reaction for PEC water splitting through decoration of plasmon metal (Ag) in a semiconductor/TMH coupling system. The kinetic behavior at the semiconductor/TMH and TMH/electrolyte interfaces is systematically evaluated by employing intensity modulated photocurrent spectroscopy, scanning photoelectrochemical microscopy, and oxygen evolution reaction model. It is found that both charge transfer and surface catalysis dynamics are enhanced through local surface plasmon resonance of Ag nanoparticles. The as‐prepared BiVO4/Co(OH)x‐Ag exhibits remarkable activity (≈4.64 times) in PEC water splitting in comparison with pure BiVO4. Notably, this smart approach can be also applied to other TMH (Ni(OH)2), reflecting its universality. This work provides a guiding design method for solar energy conversion with the semiconductor‐TMH system. [ABSTRACT FROM AUTHOR]

Combining fluorescent test strip with an easy-to-access Color Recognition App on a smartphone, the direct visualization and reliable quantitative analysis of DPA was realized based on Eu3+-functionalized copper nanoclusters. • A dual-channel luminescent signal readout probe for sensitive, rapid, and on-the-spot determination of DPA was developed. • The probe demonstrated a detection limit down to 8 nM was achieved, which is far below the infectious dose of the spores. • The combination of test paper and smartphone provided a convenient approach for visual detection of DPA. • The practical application of GSH-Cu NCs/Eu3+ was successfully exploited for DPA determination in real human serum samples. 2,6-pyridinedicarboxylic acid (DPA), as a unique biomarker of Bacillus anthracis , is highly toxic at trace levels and its pollution has shown great biological threat to homeland security and public safety worldwide. Developing portable and direct read-out devices is an inevitable trend in high demand for reliable point-of-care detection of DPA. We herein report a dual-channel luminescent signal readout probe for sensitive, rapid, and on-the-spot determination of DPA. The developed probe demonstrated a detection limit down to 8 nM was achieved, which is far below the infectious dose of the spores (60 μ M). Integrated with the low-cost paper-based sensing devices fabricated by the probe, the smartphone platform installed with a Color Recognition App could accomplish visual DPA detection, which offers a great promise for the point-of-care detection with the merits of low-cost and convenient, thus opening a new pathway for the on-site self-assessment of homeland security and public safety, especially in resource-poor settings. It is believed that the proposed assay could afford experience for designing of smart chemical nose/tongue sensor in hazardous substances monitoring. [ABSTRACT FROM AUTHOR]

Temperature regulation can not only achieve "fast" surface catalytic reaction at solid/electrolyte interface but also obtain "high" interfacial charge transport kinetics at solid/solid interface. The desired photoelectrochemical performance can be achieved by temperature regulation, but the nature for this improvement remains a controversial topic. Herein, we employed BiVO 4 /CoO x as a typical model system, and explored the fate of photogenerated holes at the different interfaces among BiVO 4 /CoO x /electrolyte by means of intensity modulated photocurrent spectroscopy (IMPS), scanning photoelectrochemical microscopy (SPECM) and traditional electrocatalysis characterization methods. Systematic quantitative analysis of the kinetics of photogenerated holes transfer at the BiVO 4 /CoO x interface under illumination and surface water oxidation at the CoO x /electrolyte interface in the dark indicates that increasing temperature could not only enhance the surface catalytic reaction kinetics but also facilitate the interfacial charge transfer. As expected, the integrated system exhibited a remarkable photocurrent density of 3.6 mA cm−2 (1.23 V RHE , AM 1.5G, 45 °C), which is approximately 2.1 times higher than that of BiVO 4 /CoO x (15 °C). This work provides a promising strategy for achieving efficient photoelectrochemical water splitting. [ABSTRACT FROM AUTHOR]

By a facile peripheral decoration of 5‐(4‐aminophenyl)‐10,15,20‐triphenylporphyrin (ATPP) with inherent aggregation‐induced emission (AIE) active tetraphenylethene (TPE), a versatile AIEgenic porphyrin derivative (ATPP‐TPE) was obtained, which greatly abolishes the detrimental π–π stacking and thus surmounts the notorious aggregation‐caused quenching (ACQ) effect of ATPP in aqueous phase. The photoluminescence of ATPP‐TPE is 4.5‐fold stronger than ATPP at aggregation state. Moreover, an unequivocal aggregation induced electrochemiluminescence (AIECL) of ATPP‐TPE was found to be seriously dependent on its aggregation property in aqueous solution with efficiency of 34 %, which is 6 times higher than pure ATPP. The versatility of this molecular structure modulation strategy along with the ACQ‐to‐AIE transformation in this work provides direction to guide for applying liposoluble porphyrins in aqueous phase by designs of synthetic porphyrin AIEgens. [ABSTRACT FROM AUTHOR]

By a facile peripheral decoration of 5‐(4‐aminophenyl)‐10,15,20‐triphenylporphyrin (ATPP) with inherent aggregation‐induced emission (AIE) active tetraphenylethene (TPE), a versatile AIEgenic porphyrin derivative (ATPP‐TPE) was obtained, which greatly abolishes the detrimental π–π stacking and thus surmounts the notorious aggregation‐caused quenching (ACQ) effect of ATPP in aqueous phase. The photoluminescence of ATPP‐TPE is 4.5‐fold stronger than ATPP at aggregation state. Moreover, an unequivocal aggregation induced electrochemiluminescence (AIECL) of ATPP‐TPE was found to be seriously dependent on its aggregation property in aqueous solution with efficiency of 34 %, which is 6 times higher than pure ATPP. The versatility of this molecular structure modulation strategy along with the ACQ‐to‐AIE transformation in this work provides direction to guide for applying liposoluble porphyrins in aqueous phase by designs of synthetic porphyrin AIEgens. [ABSTRACT FROM AUTHOR]

Surface recombination at the photoanode/electrolyte junction seriously impedes photoelectrochemical (PEC) performance. Through coating of photoanodes with oxygen evolution catalysts, the photocurrent can be enhanced; however, current systems for water splitting still suffer from high recombination. We describe herein a novel charge transfer system designed with BiVO4 as a prototype. In this system, porphyrins act as an interfacial‐charge‐transfer mediator, like a volleyball setter, to efficiently suppress surface recombination through higher hole‐transfer kinetics rather than as a traditional photosensitizer. Furthermore, we found that the introduction of a "setter" can ensure a long lifetime of charge carriers at the photoanode/electrolyte interface. This simple interface charge‐modulation system exhibits increased photocurrent density from 0.68 to 4.75 mA cm−2 and provides a promising design strategy for efficient photogenerated charge separation to improve PEC performance. [ABSTRACT FROM AUTHOR]

Surface recombination at the photoanode/electrolyte junction seriously impedes photoelectrochemical (PEC) performance. Through coating of photoanodes with oxygen evolution catalysts, the photocurrent can be enhanced; however, current systems for water splitting still suffer from high recombination. We describe herein a novel charge transfer system designed with BiVO4 as a prototype. In this system, porphyrins act as an interfacial‐charge‐transfer mediator, like a volleyball setter, to efficiently suppress surface recombination through higher hole‐transfer kinetics rather than as a traditional photosensitizer. Furthermore, we found that the introduction of a "setter" can ensure a long lifetime of charge carriers at the photoanode/electrolyte interface. This simple interface charge‐modulation system exhibits increased photocurrent density from 0.68 to 4.75 mA cm−2 and provides a promising design strategy for efficient photogenerated charge separation to improve PEC performance. [ABSTRACT FROM AUTHOR]

Highly efficient detection in the aqueous phase for water‐insoluble organic molecule probes is challenging. The bright aggregated‐state electrochemiluminescence (ECL) of 1,1‐disubstituted 2,3,4,5‐tetraphenylsiloles by a co‐reactant approach was discovered, and a heterogeneous aggregation‐induced emission ECL (HAIE‐ECL) was constructed at the electrode surface, showing very high ECL efficiency (37.8 %) and selective recognition for industrially important DNBP plasticizer with a low detection limit of 0.15 nm in the water phase. A mechanistic study indicates that ECL is mainly generated due to the high electron affinity of siloles and restriction of the intramolecular motions caused by their propeller‐like noncoplanar structures. This system realizes the sensing of organic‐based ECL in the water phase by solving the crucial problems of water insolubility and aggregation‐caused quenching (ACQ), and demonstrates potential for further application because of its design and high efficiency. A heterogeneous aggregation‐induced emission electrochemiluminescence (HAIE‐ECL) system with high ECL efficiency has been developed according to the AIE strategy. This system can detect a widely used plasticizer, DNBP, in the aqueous phase, and solve water insolubility and aggregation‐caused quenching (ACQ) in small organic molecule probe systems. [ABSTRACT FROM AUTHOR]

Highly efficient detection in the aqueous phase for water‐insoluble organic molecule probes is challenging. The bright aggregated‐state electrochemiluminescence (ECL) of 1,1‐disubstituted 2,3,4,5‐tetraphenylsiloles by a co‐reactant approach was discovered, and a heterogeneous aggregation‐induced emission ECL (HAIE‐ECL) was constructed at the electrode surface, showing very high ECL efficiency (37.8 %) and selective recognition for industrially important DNBP plasticizer with a low detection limit of 0.15 nm in the water phase. A mechanistic study indicates that ECL is mainly generated due to the high electron affinity of siloles and restriction of the intramolecular motions caused by their propeller‐like noncoplanar structures. This system realizes the sensing of organic‐based ECL in the water phase by solving the crucial problems of water insolubility and aggregation‐caused quenching (ACQ), and demonstrates potential for further application because of its design and high efficiency. [ABSTRACT FROM AUTHOR]

Trivalent organophosphorus luminophores attract considerable interest in life analysis due to their rich reactivity and wonderful life compatibility, but instability and aggregation-caused emissive quenching (ACQ) still hamper their practical applications. Herein, we report an air-stable trivalent phosphorus-embedded 1,2,3,4,5-pentaphenylphosphole (PPP) stabilized by a propeller-like noncoplanar chemical structure. Benefiting from its inherent strong aromaticity as well as the restriction of the intramolecular motions, PPP exhibits excellently aggregation-induced photoluminescence (PL) and electrochemiluminescence (ECL). Importantly, this work represents the first example of the organophosphorus ECL system that can highly detect the reactive oxygen species hypochlorous acid with a relatively lower detection limit as 8.5 nM, and highlights the promotion of aromaticity on ECL as well. [Display omitted] • Air-stable phosphole was stabilized by a propeller-like noncoplanar structure. • Phosphole could feature excellently aggregation-induced electrochemiluminescence. • High aromaticity was an important factor for enhancing the ECL performance. • Ultrasensitive detection of hypochlorous acid was achieved by such ECL system. [ABSTRACT FROM AUTHOR]

MicroRNAs are short noncoding regulatory RNAs that are increasingly used as disease biomarkers. Rapid, sensitive, and quantitative microRNAs detection methods with high specificity are imperative. Here, we for the first time developed a DNA-functionalized metal-organic framework (MOF)-based ratiometric fluorescent probe using the interaction between Thiazole Orange (TO) dye and Rhodamine B(RhB) dye molecules, and achieved sensitive detection and imaging of miRNA-21 in living cells. Among them, DNA was successfully conjugated with MOF through the Zr-O-P bond in a single step with high efficiency. Based on this ratiometric fluorescent probe, picomolar limit detection (57 pM) for miRNA-21 can be obtained without signal amplification. After penetration into the cell, intracellular miRNA-21 can also be imaged by strand-displacement reaction, even distinguishing cancer cells from normal cells was achieved. This work paves the way for the development of DNA-functionalized MOF for intracellular molecules analysis and is of great significance for the early disease diagnosis. [Display omitted] • Ratiometric fluorescent probe was constructed based on the interaction between Thiazole Orange and Rhodamine B molecules. • DNA molecules were efficiently linked to the metal-organic frameworks (MOFs) surface through Zr-O-P bonds in one step. • The developed probe demonstrated a detection limit down to 57 pM was achieved without signal amplification strategy. • The developed probe can be used for miRNA-21 imaging in different types of cells. [ABSTRACT FROM AUTHOR]

The coordination polymer [Cd(HL)(BPDA)] n · nH2O ( 1) based on 3-(5-(pyridin-4-yl)-1 H-1,2,4-triazol-3-yl)pyridine (HL) and 1,1′-biphenyl-4,4′-dicarboxylic acid (H2BPDA) was hydrothermally synthesized and characterized by single-crystal X-ray diffraction, XRPD, IR spectroscopy, and elemental analysis. The asymmetric unit of compound 1 consists of one crystallographically independent CdII ion, one HL ligand, 'two half' BPDA2- ligand, and one lattice water molecule. There are two crystallographically different BDPA2- moieties, but each of them is placed in a symmetry element. The BPDA2- ligands and CdII ions connected to2D sheet, and the 2D sheets are connected to a 3D MOF by the HL ligands. Each dimeric CdII unit links six nearest neighbors through the BPDA2- and HL ligands, and the dimeric CdII units are centrosymmetric. Two parallel HL ligands connect two dimeric CdII units, generating long Cd2-HL-Cd2-HL rings, also centrosymmetric. So we can define the dimeric CdII unit as a 6-connected node. Thus, the 3D structure can be described as a threefold parallel interpenetrated bsn beta-Sn topology. In addition, the optical properties of compound 1 and the free ligand H L were investigated. [ABSTRACT FROM AUTHOR]

Highlights: [•] A rare copper cyanide coordination polymer has been hydrothermally synthesized. [•] A ({6.8.10}2{6.8^3.10^2}) topology in 1 is created. [•] The existence of a cyanide group in compound 1 may be due to the decomposition of acetonitrile. [•] The optical and catalytic properties have been investigated. [ABSTRACT FROM AUTHOR]

A new coordination polymer, [Co2(L)2(4,4′-bipy)] n·3 nH2O ( 1) based on 5-(3-methyl-5-phenyl-4 H-1,2,4-triazol-4-yl)isophthalic acid (H2 L) and 4,4′-bipyridine (4,4′-bipy) has been hydrothermally synthesized and characterized by single-crystal X-ray diffraction, XRPD, IR, and elemental analysis. Temperature-dependent magnetic susceptibility and thermal degradation for 1 were also studied. The asymmetric unit of compound 1 consists of two crystallographically independent Co(II) ion, two L2− ligand, one 4,4′-bipy ligand, and three lattice water molecules. The 2D triangle networks were linked by the bridging 4,4′-bipy ligand to give rise to a 2-fold interpenetrated 3D architecture. The simplest cyclic motif of the 2D networks is a triangle ring consisting of three Co(II) cations and three L2− ligands. So we can define Co(II) ions as 4-connected nodes and the L2− ligands as 3-connected nodes. Thus, the 3D structure can be described as a 2-fold parallel interpenetrated ins InS 3,4-conn topology. [ABSTRACT FROM AUTHOR]

Abstract: A series of novel lanthanide-based coordination polymers, [Ln(L)(atpa)(H2O)2]n·1.5nH2O (HL =4-[3-methyl-5-(pyridin-4-yl)-1,2,4-triazol-4-yl]benzoic acid, H2atpa=2-aminoterephthalic acid and Ln=Tb(1), Dy(2), Ho(3), Er(4), Tm(5), Yb(6)) have been hydrothermally synthesized and characterized by single-crystal X-ray diffraction, optical and magnetic measurements. Compounds 1–6 are isomorphous, which can be described as a 2D network based on Ln2(CO2)2 units. The magnetic properties of compound 1 (Tb) show typical antiferromagnetic interaction, while compound 2 (Dy) has ferromagnetic behavior. The room-temperature photoluminescence spectra of 1 exhibit strong characteristic emissions in the visible region, whereas compounds of Dy(2), Er(4) and Yb(6) display NIR luminescence upon irradiation at the ligand band. [Copyright &y& Elsevier]

To keep fast proliferation, tumor cells are exposed to higher oxidative stress than normal cells and they upregulate the amount of some antioxidants such as glutathione (GSH) against reactive oxygen species to maintain the balance. This phenomenon is severe in hypoxic tumor cells. Although researchers have proposed a series of treatment strategies based on regulating the intracellular reactive oxygen species level, few of them are related to the hypoxic tumor. Herein, a novel organic compound (PLC) was designed by using lysine as a bridge to connect two functional small molecules, a hypoxia-responsive nitroimidazole derivative (pimonidazole) and a pH-responsive cinnamaldehyde (CA) derivative. Then, the oxidative stress amplifying ability of PLC in hypoxic tumor cells was evaluated. The acidic microenvironment of tumor can trigger the release of CA to produce reactive oxygen species. Meanwhile, large amount of nicotinamide adenine dinucleotide phosphate (NADPH) can be consumed to decrease the synthesis of GSH during the bio-reduction process of the nitro group in PLC under hypoxic conditions. Therefore, the lethal effect of CA can be amplified for the decrease of GSH. Our results prove that this strategy can significantly enhance the therapeutic effect of CA in the hypoxic tumor cells. [Display omitted] [ABSTRACT FROM AUTHOR]

• The synergy between surface geometry and surface electronic structure gives bimetallic nanoparticles unique properties. • The enhanced peroxidase mimetic activity by Hg–stimulated Cr@Ag NPs was used to construct a sensitive colorimetric sensor. • The developed colorimetric assay platform exhibits satisfying performances in real water samples. Metastable precious metal nanoparticles as precursors and self-templates with uniform atomic distribution provide unlimited possibilities for the construction of nano-secondary materials. Bimetallic nanomaterials with unexpected physical and chemical properties can be fabricated through a metal ion-mediated strategy. However, the interior functionalization of metastable precious metal nanoparticles so as to achieve synergistic interaction between precursors and external ions thus enhance the performance of bimetallic nanomaterials remains a challenge. Herein, the metal ion-mediated bimetallic nanomaterials such as Cr@Ag NPs, Ni@Ag NPs, Mn@Ag NPs, Cd@Ag NPs, and Pb@Ag NPs were precisely constructed on the basic of the seeds of silver nanoparticles (Ag NPs). More importantly, the integrated bimetallic nanomaterials Cr@Ag NPs could serve as the potential mimetic-peroxidase to sensitively and rapid identify Hg2+ in TMB-H 2 O 2 systems. Furthermore, the developed colorimetric assay platform exhibits satisfying performances in real water samples. The present study opens a new horizon for the design and construct novel nanomaterials with extraordinary opto-physical and chemical properties in colorimetric sensing. [ABSTRACT FROM AUTHOR]

• 3D Fe-Mn-O NSs/WC hybrid is constructed for Fenton-like oxidation. • Surface properties of Fe-Mn-O NSs are improved by doping alien-metal ions. • The catalyst shows good activity due to synergy effect of nanosheet and carrier. • Fe-Mn-O NSs/WC can be extended to a filter membrane for flowing water treatment. Cost-effective, highly efficient and conveniently recycled heterogeneous catalyst is urgently desirable for wastewater treatment. Wood-derived monolith offers new opportunity because of its toilless functionalization and flexible processing. Herein, ferrum manganese oxide nanosheets (Fe-Mn-O NSs) were successfully grown on the microchannels of carbonized wood to construct a novel 3D wood-derived block for efficient wastewater treatment. The wood carbon not only acts as a 3D substrate to support Fe-Mn-O NSs, but also contributes to unimpeded mass diffusion benefiting from the numerous open channels and hierarchical pores on channel walls. More importantly, except for the exposure of sufficient active sites, several important surface properties (i.e. surface defects, surface charge, low-valence metal concentration and charge transfer) were improved by doping alien-metal element, resulting in greatly improved Fenton activity and stability. Notably, due to flexible processing of wood carbon, this block catalyst can be extended to filter membrane for removing pollutants in flow wastewater. [ABSTRACT FROM AUTHOR]

The cover page of the journal "Chinese Journal of Chemistry" is presented.