Latest ArticlesAccurate detection of important biomarkers with ultra-low levels in complex biological matrix is one of the frontier scientific issues because of possible signal interference of potential reductive agents and protein molecules. Herein, a self-powered anti-interference photoelectrochemical (PEC) immunosensor was explored for sensitive and specific detection of model target of cardiac troponin I (cTnI). Specifically, a novel ternary heterojunction served as the photocathode to offer a remarkable current output and a zwitterionic peptide was introduced to build a robust antifouling biointerface. CuInS2 (CIS) film with porous network nanostructure was first prepared and then modified in order with ZnIn2S4 (ZIS) nanocrystals and Au nanoparticles to fabricate the Au/ZIS/CIS heterojunction photocathode. After capture cTnI antibody (Ab) was immobilized, the zwitterionic peptide KAEAKAEAPPPPC was then anchored to compete the immunosensor. The elaborated PEC immunosensor exhibited high sensitivity for target cTnI antigen (Ag) detection, with good anti-interference against reductive agents and nonspecific proteins. This integration strategy of heterojunction photocathode with zwitterionic peptide provides a new sight to develop advanced PEC immunosensors applying in practical biosamples.
Molecular oxygen (O2) is activated to reactive oxygen species (ROS) by transferring energy and carriers in the photocatalytic process, which plays an important role in environmental remediation. Herein, Cs-doped carbon nitride (CN-xCs, x = 0.2, 0.8, 1) was prepared by CsCl directly inducing the structural reconstruction of carbon nitride (CN), which had obvious molecular oxygen activation ability to promote tetracycline (TC) degradation. Besides, we explored the influence of Cs doping concentration. As a consequence, the doping concentration of Cs was an important factor affecting the activation of O2, which could cause changes in the physical and chemical structure of CN, make O enter the CN structure, form N vacancy defects and cyano groups. In addition, a proper amount of Cs doping could reduce the band gap value, increase the light absorption range, have better charge separation and transfer performance, which could remarkably promote the activation of O2. Benefiting from these advantages, CN-0.8Cs could generate a higher concentration of superoxide radicals (•O2−, 179.30 µmol/L), which was much higher than CN (6.22 µmol/L). Therefore, it exhibited excellent TC degradation photocatalytic performance, and the rate constant k of TC degradation was 0.020 min−1, which was 6.7 times the degradation rate of CN (k = 0.0030 min−1). Furthermore, the possible degradation pathways of TC were proposed based on the results of HPLC-MS.
Typically, rational interfacial engineering can effectively modify the adsorption energy of active hydrogen molecules to improve water splitting efficiency. NiFe layered double hydroxide (NiFe LDH) composite, an efficient oxygen evolution reaction (OER) catalyst, suffers from slow hydrogen evolution reaction (HER) kinetics, restricting its application for overall water splitting. Herein, we construct the hierarchical MoS2/NiFe LDH nanosheets with a heterogeneous interface used for HER and OER. Benefiting the hierarchical heterogeneous interface optimized hydrogen Gibbs free energy, tens of exposed active sites, rapid mass- and charge-transfer processes, the MoS2/NiFe LDH displays a highly efficient synergistic electrocatalytic effect. The MoS2/NiFe LDH electrode in 1 mol/L KOH exhibits excellent HER activity, only 98 mV overpotential at 10 mA/cm2. Significantly, when it assembled as anode and cathode for overall water splitting, only 1.61 V cell voltage was required to achieve 10 mA/cm2 with excellent durability (50 h).
In this work, the removal of 2,4,6-tribromophenol (TBP) by ferric ion-activated sulfite [Fe(III)/S(IV)] process was systematically investigated with determining the intermediate products and evaluating the influences of some operational conditions and water matrices. Our results show that batching addition of S(IV) benefits the S(IV) utilization efficiency and TBP removal, with SO4•‒ being the primary reactive radical accounting for TBA degradation. The maximum TBP removal in the Fe(III)/S(IV) process was observed at pH 4.0 and oxygen is essential in this process. With increasing Fe(III) and S(IV) dosages from 0.05 and 0.1 mmol/L to 0.2 and 2.0 mmol/L, respectively, TBP removal followed trends of first increase then decrease. As the acute toxicity of the TBP solution was significantly reduced, the Fe(III)/S(IV) process was believed to be a good choice in the treatment of TBP.
Formaldehyde (HCHO) causes increasing concerns due to its ubiquitously found in indoor air and being irritative and carcinogenic to humans. Photothermal-catalysis developed in recent years has been considered as a significant strategy for enhancing catalytic activity. Manganese oxides, compared with its strong thermocatalytic activity, generally suffer from much lower photocatalytic activity make its photochemical properties less concerned. Herein, α-MnO2 nanowires were composited with the graphene oxide (GO) via mechanical grinding and co-precipitating method, respectively. α-MnO2/GO nanohybrids prepared by co-precipitating method exhibits excellent activity, achieving 100% decomposition of HCHO with the solar-light irradiation at ambient temperature. It is found that, besides the photo-driven thermocatalysis, the photocatalysis mechanism made a major contribution to the decomposition of HCHO. The incorporation of GO, on the one hand, is beneficial to improve the optical absorption capacity and photothermal conversion efficiency; on the other hand, is conductive to electron transfer and effective separation of electrons and holes. These synergistic effects significantly improve the catalytic activity of α-MnO2/GO nanohybrids. This work proposes a new approach for the utilization of solar energy by combining manganese oxides, and also develops an efficient photothermal-catalyst to control HCHO pollution in indoor air.
Zn2Ti3O8, as a new type of anode material for lithium-ion batteries, is attracting enormous attention because of its low cost and excellent safety. Though decent capacities have been reported, the electrochemical reaction mechanism of Zn2Ti3O8 has rarely been studied. In this work, a porous Zn2Ti3O8 anode with considerably high capacity (421 mAh/g at 100 mA/g and 209 mAh/g at 5000 mA/g after 1500 cycles) was reported, which is even higher than ever reported titanium-based anodes materials including Li4Ti5O12, TiO2 and Li2ZnTi3O8. Here, for the first time, the accurate theoretical capacity of Zn2Ti3O8 was confirmed to be 266.4 mAh/g. It was also found that both intercalation reaction and pseudocapacitance contribute to the actual capacity of Zn2Ti3O8, making it possibly higher than the theoretical value. Most importantly, the porous structure of Zn2Ti3O8 not only promotes the intercalation reaction, but also induces high pseudocapacitance capacity (225.4 mAh/g), which boosts the reversible capacity. Therefore, it is the outstanding pseudocapacitance capacity of porous Zn2Ti3O8 that accounts for high actual capacity exceeding the theoretical one. This work elucidates the superiorities of porous structure and provides an example in designing high-performance electrodes for lithium-ion batteries.
Developing high-efficiency and robust durability electrocatalyst for hydrogen evolution reaction (HER) in water electrolysis functions as a crucial role for the construction of green hydrogen economy, herein, ultrafine W-doped vanadium nitride nanoparticles anchored on N-doped graphitic carbon framework (WVN@NGC) are synthesized through a one-step simple pyrolysis protocol. Owing to the enlarged catalytically active sites, enhanced electrical conductivity and optimized electronic structure, the resultant VN/WN@NGC delivered the prominent HER performance with overpotentials of 143 mV and 158 mV at 10 mA/cm2 in acid and alkaline media, respectively, accompanied by the long-term stability for at least 50 h. This work highlights a novel strategy for a metal-triggered modulation of nitride-based HER electrocatalyst for sustainable energy conversion device.
Bromate formation has been found in the SO4•−-based oxidation processes, but previous studies primarily focused on the bromate formation in the homogeneous SO4•−-based oxidation processes. The kinetics and mechanisms of bromate formation are poorly understood in the heterogeneous SO4•−-based oxidation processes, although which have been widely studied in the eliminations of micropollutants. In this work, we found that the presence of CuO, a common heterogeneous catalyst of peroxymonosulfate (PMS), appreciably enhanced the bromate formation from the oxidation of bromide by PMS. The conversion ratio of bromide to bromate achieved over 85% within 10 min in this process. CuO was demonstrated to play a multiple role in the bromate formation: (1) catalyzed PMS to generate SO4•−, which then oxidizes bromide to bromate; (2) catalyzed the formed free bromine to disproportionate to bromate; (3) catalyzed the formed free bromine to decomposed back into bromide. In the CuO-PMS-Br system, bromate formation increases with increasing CuO dosages, initial CuO and bromide concentrations, but decreases with increasing bicarbonate concentrations. The presence of NOM (natural organic matter) resulted in a lower formed bromate accompanied with organic bromine formation. Notably, CuO catalyzes PMS to transform more than 70% of initial bromide to bromate even after recycled used for six times. The formation of bromate in the PMS catalysis by CuO system was also confirmed in real water.
Heterogeneous transition metal catalysts are indispensable in improving environmental pollution. However, their fabrication is often costly and cumbersome, and they can easily pollute the environment. This study proposed using a natural Gabonese ore (GBO) containing MnxOy and FexOy as catalysts to degrade orange Ⅱ (OII) via peroxymonosulfate (PMS) activation. The GBO + PMS system exhibited extraordinarily high stability and catalytic activity towards OII elimination (92.2%, 0.0453 min−1). The reactive oxygen species (ROS) generated in the system were identified using radical scavenging tests and electron spin-resonance (ESR) analysis. Singlet oxygen (1O2) represented the dominant reactive species for OII degradation, while the system presented a lower reaction energy barrier and was effective in a broad pH range (2–10). This work also proposed the activation mechanism for the GBO + PMS system and OII degradation pathways. This study revealed a new approach for exploring inexpensive, eco-friendly, efficient, and stable heterogeneous transition metal catalysts.
A dual emission sensing film has been prepared for colorimetric temperature sensing using CsPbBr3 perovskite nanocrystals (CsPbBr3 NCs) and manganese doped potassium fluorosilicate (K2SiF6: Mn4+, KSF) encapsulated in polystyrene by a microencapsulation strategy. The CsPbBr3-KSF-PS film shows good temperature sensing response from 30 ℃ to 70 ℃, with a relative temperature sensitivity (Sr) up to 10.31% ℃−1 at 45 ℃. Meanwhile, the film maintains more than 95% intensity after 6 heating-cooling cycles and keeps its fluorescence characteristics after 3 months. The film can be used to monitor temperature change by naked eye under a UV lamp. In particular, the temperature discoloration point of the sensing film can be controlled by the ratio change of CsPbBr3: KSF to expand its applications. The study of the CsPbBr3-KSF-PS sensing mechanism in this work is helpful to provide effective strategies for the design of reliable, high sensitivity and stable temperature sensing system using CsPbBr3 NCs.
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