Journal of Environmental Sciences
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2019
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IF 3.556
Hanlu Shi,Rui He,Lei Sun,Gang Cao,Xiangjuan Yuan,Dongsheng Xia
A series of functional organic–metal AgCl-decorated graphitic carbon nitride (AgCl-CN x ) composites were synthesized and applied for the degradation of oxalic acid (OA) under visible light. The highest photocatalytic activity was achieved with AgCl decoration ratio of 1.0 (denoted as AgCl-CN 1.0 ). The pseudo-first-order constant for OA degradation was 0.0722 min −1 with the mineralization efficiency of 90.80% after 60 min reaction in the photocatalytic process with AgCl-CN 1.0 . A variety of characterization techniques including Brunauer–Emmett–Teller, X-ray diffraction, scanning electron microscope , transmission electron microscopy , X-ray photoelectron spectroscopy, Fourier transform infrared spectra , ultraviolet–visible diffuse reflectance spectra, photoluminescence , and Mott–Schottky were utilized to elucidate the physicochemical, microstructure, and optical properties contributing to the improvement of the photocatalytic performance. The results showed that AgCl-CN 1.0 had an oblate flaky erythrocyte-like structure with a moderate band gap energy of ~ 3.00 eV. In addition, the effects of the key parameters (i.e., AgCl-CN 1.0 dosage, initial OA concentration, solution pH, and presence of natural organic matter) on OA degradation were systematically investigated. Radical scavenger experiments indicated that photogenerated holes, electrons, superoxide anion radicals, and hydroxyl radicals were the dominant reactive species. Moreover, AgCl-CN 1.0 exhibited excellent stability and reusability for OA degradation without detectable Ag + release in the solution over multiple reaction cycles. The efficient OA mineralization could be mainly ascribed to the moderate specific surface area, increased numbers of active sites, and effective interfacial charge transfer of AgCl-CN 1.0 . Overall, the AgCl-CN 1.0 composite was demonstrated to be a highly efficient, stable, and recoverable photocatalyst.
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Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 10
·5324-5332
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IF 10.733
Mao Wu,Yansheng Gong,Tao Nie,Jin Zhang,Rui Wang,Huanwen Wang,Beibei He
Nanocage-like 3D porous graphitic carbon nitride (g-C3N4) with a high surface area and nitrogen defects was successfully prepared via a novel, template-free, cost-effective and hydrothermal-copolymerization route. Compared with pristine g-C3N4, the synergetic effect of nitrogen vacancies combined with a nanocage-like structure endowed it with a broad visible-light-responsive range, more exposed active lateral edges and catalytically active sites, as well as efficient separation of photogenerated carriers. As a consequence, the modified g-C3N4 exhibited prominent photocatalytic performance in water splitting for the hydrogen evolution reaction under visible light illumination. The optimized photocatalyst (DCN-550) showed a maximum photocatalytic H2 evolution rate of 92.57 μmol h−1, almost 20.3 times higher than that of pristine g-C3N4. Moreover, a possible mechanism for the photocatalytic hydrogen evolution and nanostructure formation process based on the experimental results was proposed. The new growth strategy developed here could inspire similar attempts to modify novel visible-light-driven photocatalysts through nanostructure design.
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ANALYTICAL CHEMISTRY
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2019
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IF 6.35
Jianguo Xu,Chao Yan,Xinxin Wang,Bangben Yao,Jianfeng Lu,Guodong Liu,Wei Chen
Facile and efficient assembly of intelligent DNA nano-objects with the ability to exert robust microRNA determination is essential for DNA nanobiotechnology and basic biomedical study. Herein, we present a novel target-triggered DNA assembly pathway for the construction of multibranched DNA nanoarchitectures by the combination of DNA concatamers with G-quadruplex wires. The DNA concatamers acting as the main body structures were assembled by hybridization chain reaction (HCR), while the G-quadruplex wires acting as the branch structures were generated by terminal deoxynucleotidyl transferase (TdT)-promoted polymerization and G-quadruplex units (GUs) based self-assembly. With a copious number of G-quadruplex replicates collected on the electrode surface, the obtained multibranched DNA nanoarchitectures were able to bind with lots of hemin, which further led to a significantly amplified electrochemical sensing signal for ultrasensitive and selective detection of miRNA-21. The detection limit was achieved as low as 0.2 fM with a wide dynamic response ranging from 10 fM to 100 nM, which is much more powerful or at least comparable to most of the reported studies. Furthermore, the electrochemical biosensor offered an excellent specificity, and even the single-base mutation against the perfectly matched target miRNA can be easily distinguished easily. Furthermore, the real biological samples were also desirably analyzed, indicating that the proposed strategy is an ideal platform for the fabrication of versatile DNA nanobiosensors.
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REACTIVE & FUNCTIONAL POLYMERS
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2019
·
IF 3.074
Yunqing Xia,Yi He,Chunlin Chen,Youqing Wu,Fei Zhong,Jingyu Chen
In this work, the hydrophilic organic films were successfully coated on g-C 3 N 4 nanosheets through facile co-modification of dopamine (DA) and silane coupling agent (KH560). The co -modification of polydopamine (PDA) and KH560 on lamellar g-C 3 N 4 greatly enhanced dispersion of g-C 3 N 4 in aqueous solution and dramatically improved the compatibility and interfacial interaction with waterborne epoxy. The effect of incorporating modified g-C 3 N 4 nanosheets into waterborne epoxy on anticorrosion performance for P110 steel substrates were demonstrated through electrochemical impedance spectroscopy (EIS), potentiodynamic polarization and salt spray test. The results revealed that the |Z| 0.01Hz value and percentage coating resistance (R c ) gain (η c %) of nanocomposite coating increased by 977% and 90.72% with the addition of modified g-C 3 N 4 nanosheets in comparison with pure waterborne epoxy coating, exhibiting outstanding anticorrosion abilities. The reinforced anticorrosion performances of nanocomposite coating could be attributed to the notable shielding effect and well dispersibility of modified g-C 3 N 4 nanosheets.
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Nanomaterials
·
2019
·Vol. 9
·期 8
·1139
·
IF 4.034
Bo Zhang,Zhenhai Wang,Xiangfeng Peng,Zhao Wang,Ling Zhou,QiuXiang Yin
An atmospheric plasma treatment strategy was developed to prepare two-dimensional (2D) molybdenum disulfide (MoS2) and graphitic carbon nitride (g-C3N4) nanosheets from (NH4)2MoS4and bulk g-C3N4, respectively. The moderate temperature of plasma is beneficial for exfoliating bulk materials to thinner nanosheets. The thicknesses of as-prepared MoS2and g-C3N4nanosheets are 2–3 nm and 1.2 nm, respectively. They exhibited excellent photocatalytic activity on account of the nanosheet structure, larger surface area, more flexible photophysical properties, and longer charge carrier average lifetime. Under visible light irradiation, the hydrogen production rates of MoS2and g-C3N4by plasma were 3.3 and 1.5 times higher than the corresponding bulk materials, respectively. And g-C3N4by plasma exhibited 2.5 and 1.3 times degradation rates on bulk that for methyl orange and rhodamine B, respectively. The mechanism of plasma preparation was proposed on account of microstructure characterization and online mass spectroscopy, which indicated that gas etching, gas expansion, and the repulsive force of electron play the key roles in the plasma exfoliation. Plasma as an environmentally benign approach provides a general platform for fabricating ultrathin nanosheet materials with prospective applications as photocatalysts for pollutant degradation and water splitting.Keywords:dielectric barrier discharge plasma;MoS2nanosheets;g-C3N4nanosheets;photodegradation;water splitting;gas etching;repulsive force
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Ruiyang Zhang,Zeai Huang,Chengjin Li,Yisu Zuo,Ying Zhou
Photocatalysis has been known as a promising technique for environmental remediation and clean energy production. However, there are two weaknesses for photocatalyst in powder form applied in the gas-phase catalysis. One is the inadequate contact of gas pollutant as well as utilization of light energy and the other one is the intricate operations for recycle. Herein, we reported a new-type monolithic Pd-embedded g-C 3 N 4 /reduced graphene oxide aerogel (Pd-g-C 3 N 4 /RGOA) photocatalyst prepared through one-pot thermal reduction method. In this case, a synergistic effect was realized, in which g-C 3 N 4 powder was uniformly dispersed on the surface of RGOA and connected with RGOA through the formation of 2D-2D π-π conjugated structure to enhance the contact of gas pollution and utilization of light energy as well as separation of charge carriers, while Pd acted as an electron sink to promote electron-hole separation and its unique electronic structure improved the gas adsorption. As a result, the obtained Pd-g-C 3 N 4 /RGOA revealed enhanced hydrogenation of CO 2 to CH 4 with a max CH 4 evolution rate of 6.4 μmol g −1 h −1 , which is 12.8-fold enhancement than that of pure g-C 3 N 4 . This study provides a fresh insight for the design of efficient monolithic photocatalyst for gas-phase catalysis.
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ANALYTICA CHIMICA ACTA
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2018
·
IF 5.123
Yanyu Lin,Rongkai Shen,Nannan Liu,Huan Yi,Hong Dai,Jianhua Lin
Here, a simple electrochemical biosensor was proposed based on the specific recognition between trypsin and peptide. Initially, NiCo 2 O 4 -PAMAM nanocomposite was casted on the bare electrode to achieve the electrochemical signal amplification in 0.1 mM [Ru(NH 3 ) 6 ] 3+ solution owing to the great electronic conductivity and high electrochemical activity induced by the special structure of NiCo 2 O 4 nanosheets (Ni 3+ cations in octachedral sites of the Co 3 O 4 ). Subsequently, a declined electrochemical signal was obtained when g-C 3 N 4 labeled peptide composites were anchored on the electrode. However, after trypsin was added into solution and incubated with the biosensor, the electrochemical signal was re-promoted. Therefore, the as-synthesized biosensor could realize the sensitive detection of trypsin by virtue of the specific recognition between trypsin and peptide. As a result, the developed peptide-based exhibited a linear range from 10 −10 to 10 −4 mg mL −1 with an ultralow detection limit of 10 −10 mg mL −1 , providing sensitive analytical performance and acceptable application potential in clinical test and disease diagnosis due to its high stability, excellent selectivity , acceptable reproducibility and accurate signal output.
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Journal of CO2 Utilization
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2018
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IF 5.503
Qian Li,Zhuxing Sun,Haiqiang Wang,Zhongbiao Wu
In this study, hollow-structured Bi decorated g-C 3 N 4 hybrids were successfully fabricated by a simple solvothermal method and applied for the first time to the photocatalytic reduction of CO 2 . Remarkably, the composites exhibited excellent CO 2 conversion efficiencies in the presence of H 2 O under visible light irradiation compared to unmodified g-C 3 N 4 , especially for the production of CH 4 . The optimum photocatalyst 30-Bi/g-C 3 N 4 presented the best production of CO and CH 4 , approximately 3 times and 9 times as high as those of unmodified g-C 3 N 4 , respectively. A series of characterizations were conducted to explore the essence behind such an enhancement; we found that enhanced light harvesting, quick separation of photoinduced carriers and more negative conduction band, due to the formation of a Schottky junction between g-C 3 N 4 and Bi metal and the solvothermal process, co-contributed for the enhanced CO 2 conversion; A more important finding was that the surprising improvement of CH 4 yield stem primarily from the introduction of the hollow-structured Bi, which enabled the accumulation of electrons on its surface exhibiting the metal-like property. The CO 2 photocatalytic conversion process was also investigated by in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFT) spectroscopy and we found that HCO 3 − and CO 2 − were active intermediates over 30-Bi/g-C 3 N 4 and Bi doping could promote the activation of CO 2 . In summary, this work presented hollow-structured Bi decorated g-C 3 N 4 composites as new materials for energy applications, proving once more the meta-like nature of bismuth, and laying the groundwork for the utilization of Bi in CO 2 photocatalytic reduction processes.
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ACS Applied Materials & Interfaces
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2018
·
IF 8.097
Lingling Hu,Huanjunwa He,Dehua Xia,Yajing Huang,Jiarong Xu,Haoyue Li,Chun He,Wenjing Yang,Dong Shu,Po Keung Wong
A self-stabilized Z-scheme porous g-C3N4/I3–-containing BiOI ultrathin nanosheets (g-C3N4/I3–-BiOI) heterojunction photocatalyst with I3–/I– redox mediator was successfully synthesized by a facile solvothermal method coupling with light illumination. The structure and optical properties of g-C3N4/I3–-BiOI composites were systematically characterized by means of X-ray diffraction, scanning electron microscopy, transmission electron microscopy, Fourier transform infrared, X-ray photoelectron spectroscopy, N2 adsorption/desorption, UV–vis diffuse reflectance spectrum, and photoluminescence. The g-C3N4/I3–-BiOI composites, with a heterojunction between porous g-C3N4 and BiOI ultrathin nanosheets, were first applied for the photocatalytic elimination of ppm-leveled CH3SH under light-emitting diode visible light illumination. The g-C3N4/I3–-BiOI heterojunction with 10% g-C3N4 showed a dramatically enhanced photocatalytic activity in the removal of CH3SH compared with pure BiOI and g-C3N4 due to its effective interfacial charge transfer and separation. The adsorption and photocatalytic oxidation of CH3SH over g-C3N4/I3–-BiOI were deeply explored by in situ diffuse reflectance infrared Fourier transform spectroscopy, and the intermediates and conversion pathways were elucidated and compared. Furthermore, on the basis of reactive species trapping, electron spin resonance and Mott–Schottky experiments, it was revealed that the responsible reactive species for catalytic CH3SH composition were h+, •O2–, and 1O2; thus, the g-C3N4/I3–-BiOI heterojunction followed an indirect all-solid state Z-scheme charge-transfer mode with self-stabilized I3–/I– pairs as redox mediator, which could accelerate the separation of photogenerated charge and enhance the redox reaction power of charged carriers simultaneously.
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ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Dong Yang,Yishan Zhang,Hongjian Zou,Shaohua Zhang,Yizhou Wu,Ziyi Cai,Jiafu Shi,Zhongyi Jiang
Nicotinamide cofactors (e.g., NADH) are essential hydrogen sources for the majority of enzyme reduction reactions. Currently, highly efficient and in situ cofactor regeneration is urgently required but remains challenging. In this study, red phosphorus quantum dots were decorated onto graphitic carbon nitride hollow tubes to prepare high-performance heterojunction photocatalyst (g-C3N4-HTs@rP-QDs) for visible-light-driven NADH regeneration. Energy band analysis combined with photoelectrochemical measurements demonstrates rP-QDs not only act as additional photosensitizers for charge generation but also constitute a type II heterojunction with g-C3N4-HTs for charge transfer, facilitating enrichment of electrons on the g-C3N4-HTs surface. Such enrichment of electrons for g-C3N4-HTs@rP-QDs offers ∼5 times higher reducing active sites than bulk g-C3N4 to trigger the NADH regeneration reaction under visible-light (LED, 405 nm) illumination, thus acquiring superior NADH regeneration efficiency with an initial reaction rate (2 min) of 0.247 ± 0.012 mmol g–1 min–1. In the concerned experimental range, higher g-C3N4-HTs/rP-QDs mass ratios or light intensities that are beneficial for the electron enrichment could result in enhanced regeneration efficiency. The bioactivity of NADH toward enzyme catalysis is further demonstrated by alcohol dehydrogenase-catalyzed hydrogenation of formaldehyde, which enables the sustainable production of methanol.
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Molecular Medicine Reports
·
2018
·Vol. 18
·期 3
·3193-3202
·
IF 1.922
Bo Yan,Dongsheng Wang,Qiang Wang,Xiaolan Lu,Qin Du,Qi Liang,Xingliang Jiang,Xiaolan Guo,Jingguo Zhou,Yan Xing
At present, the majority of methods used for uric acid (UA) detection are not able to meet the detection requirements with speed, accuracy, high sensitivity, high specificity, a wide linear range or a low cost. Compared with other methods, the electrochemical method has a high sensitivity and fast detection. The present study aimed to identify an electrochemical sensor with high sensitivity, fast detection and a wide linear range for the detection of UA. A glassy carbon electrode modified with graphene‑molybdenum disulfide‑Nafion (G‑MoS2‑Nafion) composites was prepared for use as the working electrode. The morphologies and elemental compositions of the G‑MoS2 composites were characterized by field emission scanning electron microscopy, elemental distribution spectrometry and X‑ray diffraction, respectively. The electrochemical behaviors were investigated by cyclic voltammetry, linear sweep voltammetry and the amperometric i‑t curve (i‑t). The interference of glucose, ascorbic acid and dopamine, and the accuracy and precision of the electrochemical method were subsequently evaluated. The present study identified the following: (1) Only the reduction peak of UA was detected in human serum, indicating that the method established in the present study has a high specificity for the determination of UA in human serum; (2) UA concentration has a linear correlation with current intensity (y=0.012x+0.998; R2=0.998), wide linear range and high sensitivity (minimum detectability=13.91 µM; signal‑to‑noise ratio=3); (3) the values of UA content in human serum were positively proportional to the clinical results (y=0.9802x+11.494; R2=0.978); (4) the average recovery rate of UA (95.28%) and the replicability assay of the i‑t electrochemical method (coefficient of variation=2.04%), suggest that the method had a high accuracy and good precision for UA detection. Due to its characteristics of good accuracy, high sensitivity, wide linear range, good anti‑interference ability and replicability, G‑MoS2‑Nafion has good prospects for UA detection in the clinical setting.
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CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Chao Liu,Yawei Liu,Yongqiang Guo,Chao Wang,Zhen Hu,Chunhua Zhang
In this study, a novel PA-g/co-PVP reverse osmosis (RO) composite membrane with high-hydrophilic, antifouling, high salt rejection properties, was prepared according to the principle of sand-fixing grass effect for pharmaceutical wastewater treatment. N-vinyl-2-pyrrolidone (NVP) was used as a “seed agent” that was seeped into a low cross-linked polyamide (PA) film. A hydrophilic molecular brush of polyvinylpyrrolidone (PVP) grafted on the PA surface (PA-g-PVP) similar to grass growing on sand and a cross-linked copolymer layer of PA and NVP (PA-co-NVP) similar to grass roots distributed in sand, as well as an interlayer cross-linking between PA separation layer and PES ultrafiltration membrane with a highly stable interfacial structure, synchronously occurred through γ-ray radiation. Upon incorporation of 1.0% of NVP, the resultant PA-g/co-PVP membrane achieved 18.8° water contact angle and high flux recovery ratio (FRR) values of 91.23%, 96.28%, and 93.67% for the foulants of bovine serum albumin (BSA), sodium alginate (SA), and sodium dodecyl sulfate (SDS), respectively. The FRR value of pharmaceutical wastewater-polluted membrane after cleaning was 94.30%. The PA-g/co-PVP RO membrane showed outstanding separation stability due to the radiation cross-linking reactions, which limit matrix swelling and interface delamination similar to the action principle of sand-fixing grass. These merits prove that the RO membrane developed in this study can be used in many applications, including small organic molecular wastewater separation.
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