CHEMOSPHERE
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2023
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IF 8.8
Lin Dong,Yunlan Xu,Dengjie Zhong,Haixing Chang,Jun Li,Yi Liu,Zhuofan Han
In order to develop efficient photoanode to improve the performance of visible light responsive photocatalytic fuel cell (PFC), in this work, polyaniline/g-C 3 N 4 /Bi 2 O 3 /Ti photoanode was successfully prepared using silica-sol drop coating method, and assembled with Cu cathode to construct PFC to decompose rhodamine B and generate electricity simultaneously. The degradation rate, maximum photocurrent density and maximum power density of this PFC were 91.23%, 0.086 mA cm −2 and 4.78 μW cm −2 , respectively, which were 1.4 and 1.8 times, 2.4 and 4.5 times, and 1.9 and 7.3 times those of the corresponding values of the PFCs with g-C 3 N 4 /Bi 2 O 3 /Ti and Bi 2 O 3 /Ti photoanodes, respectively. This is attributed to the type II heterojunction structure formed among polyaniline, g-C 3 N 4 and Bi 2 O 3 in the polyaniline/g-C 3 N 4 /Bi 2 O 3 /Ti photoanode. Among them, polyaniline has π-π conjugated structure, which can rapidly transfer the electronic charge between g-C 3 N 4 and Bi 2 O 3 , thus enhancing the separation efficiency of photo-generated e − -h + pairs spatially and reducing their recombination, extending the visible light response wavelength of the photocatalyst, and finally improving its photocatalytic properties. This study can provide significant reference for the research of Bi 2 O 3 -based visible light responsive PFC.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2023
·
IF 4.3
Qingyun He,Shanxi Gong,Qinghua Liang,Zhifeng Liu,Binbin Shao,Ting Wu,Yuan Pan,Xiansheng Zhang,Miao He,Lin Ge,Jingwen Sun
A novel Schottky heterojunction was obtained by co-calcining fish-scale tubular carbon nitride (FTCN), V-BiOIO 3 and Tungsten carbide (WC) for photocatalytic degradation of tetracycline hydrochloride (TCH). The novel Schottky heterojunction has been analyzed by several characterizations and experiments. The case of photocatalytic degradation was studied for different initial concentrations, electrolyte and pH, respectively. The experiments have indicated that the V-BiOIO 3 /g-C 3 N 4 /WC performed an excellent activity of photocatalytic for TCH degradation (89.0%). In the mechanism analysis, we first deduce that the V-BiO3/FTCN compound belongs to the S-scheme heterojunction photocatalysts based on the properties of the band gap structure, which can effectively suppress recombination of joint carriers. Secondly, the introduction of the cocatalyst WC formed Schottky junction, which could play a role as an electronic library to trap e − and promote the separation of photo-induced carrier and thus maximize the strong oxidation ability of h + . In addition, the introduction of WC could also significantly enhance the optical absorption properties of the composites. This research could provide a new idea for the construction of novel and efficient carbon nitride-based photocatalysts under VSL (visible light), and promote its practical application in environmental remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Qian Liu,Kangping Cui,Minshu Cui,Xueyan Liu,Qiang Zhang
Carbon substitution of nitrogen is considered as a non-toxic and stable way to improve the availability of π electrons in g-C 3 N 4 . In this paper, a simple one-step calcination method was adopted to prepare carbon and cyano co-doped g-C 3 N 4 (C-CND), photocatalytic experiments, characterization and excited state calculations showed that carbon substitution of bridging nitrogen greatly improved the π-conjugated system and synergistically modulated the electronic structure of g-C 3 N 4 with cyano, enhancing the photocatalytic activation towards peroxymonosulfate (PMS) by C-CND. Both radicals and non-radicals play an essential role in the C-CND/PMS/Vis system, where 1 O 2 dominates, and the activation mechanism is analyzed by combining the adsorption calculations between PMS and C-CND in different electrostatic potential regions. The results provide a valuable reference for the efficient photocatalytic activation of PMS by carbon self-doped g-C 3 N 4 .
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 19
·55044-55056
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IF 5.8
Bi Renke,Liu Jialong,Zhou Chutong,Shen Yijie,Liu Zhe,Wang Zhiyu
The construction of heterojunctions between semiconductors is a preferred route to improve overall photocatalytic activity. In this work, a facile and feasible method was innovatively developed to one-step prepare g-C 3 N 4 /TiO 2 heterojunctions via an absorption-calcination process using nitrogen and titanium precursors directly. This method can effectively avoid interfacial defects and establish a tight interfacial connection between g-C 3 N 4 and TiO 2 . The resultant g-C 3 N 4 /TiO 2 composites exhibited prominent photodegradation efficiency for tetracycline hydrochloride (TC-HCl) under visible light and simulated-sunlight irradiation. The optimal g-C 3 N 4 /TiO 2 composite (urea content of 4 g) showed the highest photocatalytic efficiency, which can degrade 90.1% TC-HCl under simulated-sunlight irradiation within 30 min, achieving 3.9 and 2 times increases compared to pure g-C 3 N 4 and TiO 2 , respectively. Besides, photodegradation pathways based on the role of active species ·O 2 − and ·OH were identified, indicating that a direct Z-scheme heterojunction was formed over the g-C 3 N 4 /TiO 2 photocatalyst. The enhanced photocatalytic performance can be attributed to the close-knit interface contact and the formation of Z-scheme heterojunction between g-C 3 N 4 and TiO 2 , which can accelerate the photo-induced charge carrier separation, broaden the spectra absorption range, and retain a higher redox potential. This one-step synthesis method may provide a new strategy for the construction of Z-scheme heterojunction photocatalysts consisting of g-C 3 N 4 and TiO 2 for environmental remediation and solar energy utilization.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Mingrui Guo,Meng Chen,Jixiang Xu,Chao Wang,Lei Wang
Introducing defects and heteroatoms on carbon nitride (g-C 3 N 4 , CN) framework are effective ways to enhance its photocatalytic activity by regulating light absorption and charge carriers separation. Herein, a mechanochemical method was employed to synthesize Br-doped C, N-deficient CN (CN V -mCN-Br) via ball-milling of N-containing precursor and 6-Bromopyridine-3-carbaldehyde (BrPyCHO) followed by calcining. The ball-milling-evolved mechanical forces and BrPyCHO-derived HBr induced formation of C, N vacancies and C-Br bond in CN V -mCN-Br framework. The CN V -mCN-Br exhibited curled nanosheets morphology and separated electrons-holes distribution. The photocatalytic H 2 evolution rates of 1 %Pt-loaded CN V -mCN-Br in distilled water and simulated seawater were 22.21 and 34.41 mmol g –1 h −1 , respectively with 10% triethanolamine . The corresponding apparent quantum yields were 25.87% and 40.08% at 420 nm. This work provides a facile technique to simultaneously introduce defect and heteroatom in CN for high-efficiency photocatalytic H 2 evolution.
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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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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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DYES AND PIGMENTS
·
2019
·
IF 4.018
Meng Li,Bo Wang,Xufei An,Zhiyong Li,Hongtao Zhu,Boyang Mao,David G. Calatayud,Tony D. James
A fluorescent sensor for the detection of trithiocyanuric acid (TCA) and Hg 2+ was developed based on competitive interactions: non-covalent stacking between g-C 3 N 4 and TCA vs coordinative interaction between TCA and Hg 2+ . Electrostatic simulations were used to evaluate the interactions and help describe the detection mechanism. Moreover, normalized 2D fluorescence contour plots have been used to understand the fluorescence phenomenon. When TCA was added into a g-C 3 N 4 nanosheet solution free of Hg 2+ , TCA interacted with g-C 3 N 4 nanosheets via hydrogen bonding and π-π interactions, resulting in fluorescence quenching of the g-C 3 N 4 nanosheets. However, upon the addition of Hg 2+ , the fluorescence of the TCA-g-C 3 N 4 nanosheet hybrid system was restored, due to coordination of Hg 2+ with TCA through the S atoms, breaking the TCA-g-C 3 N 4 stacking interaction. Our results provide a new approach for the design of multifunctional nanosensors suitable for the detection of environmental pollutants.
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TALANTA
·
2018
·
IF 4.244
Yue Wang,Xue Li,Geoffrey I.N. Waterhouse,Yunlei Zhou,Huanshun Yin,Shiyun Ai
In this work, a novel and sensitive photoelectrochemical (PEC) strategy was designed for protein kinase A (PKA) detection, comprising carbon microsphere (CMS) modified ITO electrode, TiO 2 as the phosphate group recognition material and graphite-carbon nitride (g-C 3 N 4 ) as photoactive material. For the first time, gold nanoparticle decorated zeolitic imidazolate frameworks (Au-ZIF-8) was employed to fabricate biosensor for PKA activity assay with the function of substrate peptide immobilization and signal amplification. Firstly, substrate peptides were assembled on the Au-ZIF-8/CMS/ITO surface through the covalent bonding between the gold nanoparticles (AuNPs) and sulfydryl groups of the peptides. Then, in the presence of ATP , phosphorylation of the substrate peptide was achieved under PKA catalysis. Finally, TiO 2 -g-C 3 N 4 composites were further modified on the electrode surface based on bonding between TiO 2 and phosphate groups created via phosphorylation of the peptide (yielding TiO 2 -g-C 3 N 4 /P-peptide/Au-ZIF-8/CMS/ITO), which is different with our previous work by directly immobilizing g-C 3 N 4 composite on electrode surface. The developed method showed a wide linear range from 0.05–50 U mL −1 . The detection limit was 0.02 U mL −1 (S/N = 3). The constructed biosensor exhibited high detection specificity for PKA. In addition, the wide applicability of this biosensor was demonstrated by evaluating the inhibition ability of ellagic acid towards PKA.
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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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Catalysis Science & Technology
·
2019
·Vol. 9
·期 14
·3753-3762
·
IF 5.726
Xianliang Qiao,Zhiqiang Zhou,Xinyu Liu,Chaoyue Zhao,Qingxin Guan,Wei Li
Graphitic carbon nitride (denoted as “g-C3N4”), as a graphite-like CN material, is widely used in catalysis. In this paper, a fragmentary g-C3N4 framework with a porous structure and rich nitrogen defects was synthesized for acetylene hydrochlorination, using melamine formaldehyde (MF) resin as an oxygen-containing precursor. The fragmentary g-C3N4 shows a highly efficient activity with acetylene conversion reaching 94.5%, which is 30 times higher than that of pure g-C3N4 prepared by direct pyrolysis of melamine. Both experimental and characterization studies by XRD, XPS and TG-MS reveal that the high activity of the catalyst is mainly derived from the porous structure and rich nitrogen defects, which are attributed to the etching of the g-C3N4 framework by oxygen species in the MF resin. Moreover, density functional theory (DFT) calculations demonstrated that the nitrogen defects in the g-C3N4 framework greatly improved the adsorption of HCl and acetylene, and at the same time significantly reduced the energy barrier from 62.0 to 38.1 kcal mol−1 at the rate-determining step.
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Journal of Environmental Sciences
·
2019
·
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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