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NEW JOURNAL OF CHEMISTRY · 2023 ·Vol. 47 ·期 14 ·6958-6966 · IF 3.3

Regulating the interfacial charge separation between MoS2 QDs and sea-urchin graphitic carbon nitride for deep photodegradation of tetracycline under visible light

Xingyu Zhan,Hao Zhang,Yunxiong Zeng,Jingcai Xu,Ao Jin,Xinqing Wang,Jing Li,Yanting Yang,Bo Hong

Graphitic carbon nitride (CN) is considered to be a promising metal-free photocatalyst, but the charge carrier separation and rapid complexation of electrons and holes are difficult to modulate for effective and comprehensive photodegradation of TC. In this work, a MoS2 QD decorated sea-urchin carbon nitride nanohybrid was prepared via a water bath method. In comparison to the 85.6% degradation efficiency of sole sea-urchin carbon nitride (SUCN), the optimized 5% MoS2 QDs/SUCN (5%MSUCN) demonstrated a removal efficiency of 96.0% towards aqueous tetracycline (TC) under visible light. Such an outstanding photoactivity was mainly attributed to the interfacial synergistic effect of MoS2 QDs and SUCN, in which the outstanding charge extraction ability and quick surface kinetics of MoS2 QDs were primarily accountable for the subsequent deep photodegradation behavior of 5%MSUCN. A series of factors that may affect photoactivity of 5%MSUCN include pH values, inorganic ions, and organic matter. Finally, the deep photodegradation mechanisms of TC and intermediates were proposed based on ex situ HPLC-MS. This work not only explains the deep decomposition of TC but also presents a facile approach for designing and manufacturing carbon nitride nanohybrids.

CAS / MDL: 7647-14-5 64-75-5
研究领域: 材料科学 · 环境科学 · 光化学
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DIAMOND AND RELATED MATERIALS · 2023 · IF 4.1

Synthesis of molybdenum trioxide/graphite carbon nitride heterojunction modified by biomass carbon dots and its application in photocatalytic degradation of methylene blue

Fenglin Tang,Jiaojiao Tang,Dan Wang,Caixia Deng,Shuang Li,Xiupei Yang

Herein, a hexagonal molybdenum trioxide/graphite carbon nitride heterojunction modified by biomass carbon dots was synthesized by a simple one-pot method and successfully applied to the degradation of methylene blue as a photocatalyst . It was confirmed that under optimal compounding conditions, graphite carbon nitride and hexagonal molybdenum trioxide combined to form a heterojunction, and the coupling interface accelerated the charge transfer efficiency. The modification of supplementary biomass carbon dots can improve the photocatalytic activity of the photocatalyst for the degradation of methylene blue. The proposed heterojunction shows better photocatalytic activity than bulk graphite carbon nitride and has good reusability and stability. After irradiation with simulated visible light for 1 h, the degradation rate of methylene blue by the heterojunction reached 67 %, which was 2.7, 2.6 and 5.8 times higher than that of bulk graphite carbon nitride, pure hexagonal molybdenum trioxide and pure carbon dots, respectively.

研究领域: 材料科学 · 环境科学
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING · 2023 · IF 4.1

Carbon quantum dot implanted graphite carbon nitride nanorod with enhanced photocatalytic activity: Mechanisms, degradation pathway and DFT calculation

Ying Zhao,Shuo Wang,Zhiqiang Sun,Qingliang Liu,Jun Ma

Graphitic carbon nitride (g-C 3 N 4 ) is recognized as a promising photocatalyst for energy and environmental remediation. However, its performance has been limited by issues such as sluggish photocarrier transfer and inadequate light absorption. To address such challenges, we fabricated an innovative photocatalyst by implanting zero-dimensional carbon quantum dots (CQDs) within one-dimensional g-C 3 N 4 nanorods . The CQD incorporation accelerated the charge separation/transfer, simultaneously, broadened the light-harvesting ability through the up-converted fluorescent properties. Density functional theory calculations were applied to gain insights into the influence of implanted CQDs on the band gap and charge behavior of CQDs/g-C 3 N 4 . Moreover, the π-π conjugation between the g-C 3 N 4 and CQD enabled the photogeneration of charge carriers. As a result, the CQDs/g-C 3 N 4 photocatalyst exhibited superb photocatalytic degradation under visible light irradiation, and the removal rates of tetracycline (TC) was 94.3%, surpassing that of pure g-C 3 N 4 by 1.2 times. Additionally, CQDs/g-C 3 N 4 processed excellent reusability and mineralization for TC degradation. The photocatalytic degradation pathway of TC was proposed using LC-MS. Mechanisms studies revealed that the photogenerated holes (h + ), hydroxyl (•OH) and superoxide radicals (•O 2 – ) were the primary reactive species responsible for driving the photodegradation process. This study provided a valuable strategy for the design of efficient and stable photocatalysts for antibiotic wastewater remediation .

CAS / MDL: 60-54-8
研究领域: 环境科学 · 材料科学
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Journal of Cleaner Production · 2021 · IF 9.297

Effects of inter/intralayer adsorption and direct/indirect reaction on photo-removal of pollutants by layered g-C3N4 and BiOBr

Fanpeng Meng,Jun Wang,Wenjie Tian,Huayang Zhang,Shaomin Liu,Xiaoyao Tan,Shaobin Wang

Photocatalysis is an effective process to utilize solar energy for contaminants degradation, and the catalytic performance depends on the intrinsic structural properties of catalysts and organic molecules as well as their interactions. This work innovatively reveals that layer-structured graphitic carbon nitride (GCN) and BiOBr exhibit distinctly different adsorption and photocatalytic behaviors and that they show respective advantages in catalytic removals of Congo red (CR) and ibuprofen (IBP). The kinetic rate constant of CR removal by GCN was about 1.3 times higher than that by BiOBr, while BiOBr has a superior photocatalytic degradation performance towards IBP with a 25-fold-higher kinetic rate constant than that of GCN. Experiments including temperature-controlled adsorption and degradation as well as mechanism discussion confirmed that IBP and CR could be strongly adsorbed in the surface intralayer of BiOBr and GCN, through unique coordination interaction, while CR adsorption on BiOBr was dominated by interlayer adsorption. Thermodynamically, we examine that these layered catalysts can induce different reactive species according to their unique valence band and conduction band locations and then trigger different oxidation pathways for degradation reaction, as confirmed by the quenching experiments. Depending on the dissociated superoxide (O 2 •− ) radical induced indirect oxidation pathway, GCN has higher kinetics for CR degradation than BiOBr. In contrast, BiOBr offers better photocatalytic performance for IBP degradation through the direct oxidation pathway of photogenerated holes (h + ). BiOCl, with an analogous structure to BiOBr, also exhibits a similar behavior to BiOBr. This work provides a new perspective for understanding the different behaviors of layer-structured materials in selective oxidation of pollutants.

研究领域: 环境科学 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2020 · IF 7.489

Facile synthesis of the Z-scheme graphite-like carbon nitride/silver/silver phosphate nanocomposite for photocatalytic oxidative removal of nitric oxides under visible light

Guojun Li,Jia Guo,Yangyun Hu,Yanan Wang,Jianbo Wang,Shule Zhang,Qin Zhong

In this study, a novel ternary Z-scheme Graphite-like Carbon Nitride (g-C 3 N 4 )/Silver (Ag)/Silver Phosphate (Ag 3 PO 4 ) photocatalyst was designed and prepared using a two-step method (sodium chloride (NaCl) template-assisted strategy plus selective deposition). Its photocatalysts performance against removing 400 ppm of Nitric Oxides (NOx) was then investigated. We found 50 wt% g-C 3 N 4 /Ag/Ag 3 PO 4 (AP-CN 2:1) catalyst removes up to 74% of NO in 90 min under the illumination of visible light (>420 nm), which is respectively 3.5 and 1.8 times higher than using g-C 3 N 4 or Ag 3 PO 4 , alone. This improved performance was attributed to the formation of Z-scheme g-C 3 N 4 /Ag/Ag 3 PO 4 heterojunction , driven by the built-in electric field across the g-C 3 N 4 /Ag/Ag 3 PO 4 interface. These separated the electron-hole but enhanced the original strong oxidation and reduction performance of related components. The superior performance is also attributed to the improved surface area, enhanced hydrophilicity (H 2 O 2 ) and better visible-light-harvesting capability of the composite compound. More importantly, the AP-CN 2:1 sample maintained a NO removal rate of more than 73% even after four rounds of recycling. The photocatalytic oxidation removal mechanism was evaluated using the radical-capture experiments, electron spin resonance (ESR) and ion-exchange high-performance liquid chromatography (HPLC) analysis. The findings of this work offer a simple but effective design of a highly reactive and practical ternary Z-scheme heterojunction photocatalysts for the removal of toxic NO.

CAS / MDL: 7647-14-5 461-58-5
研究领域: 环境科学 · 材料科学
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FUEL · 2020 · IF 5.578

Highly efficient hydrolysis of ammonia borane using ultrafine bimetallic RuPd nanoalloys encapsulated in porous g-C3N4

Yong-Ting Li,Xiao-Li Zhang,Zhi-Kun Peng,Pu Liu,Xiu-Cheng Zheng

The hydrolysis of solid storage compounds including ammonia borane (NH 3 BH 3 ) is promising for the upcoming hydrogen economy. So, developing highly efficient heterogeneous catalysts for the hydrolysis of ammonia borane is one of the key issues since this reaction is not kinetically feasible at room temperature. In this work, a facile adsorption- in situ reduction method is adopted to stabilize the ultrafine bimetallic RuPd nanoparticles on an ultrathin porous graphite carbon nitride. Due to the synergistic alloying effect, most of the resultant bimetallic Ru 1- x Pd x /g-C 3 N 4 catalysts possess much higher catalytic activity than the monometallic Ru/g-C 3 N 4 and Pd/g-C 3 N 4 in the hydrolytic dehydrogenation of ammonia borane. Catalyzed by the optimal Ru 0.85 Pd 0.15 /g-C 3 N 4 , the turnover frequency and the apparent activation energy are 948.2 mol H 2 ·mol Cat -1 ·min - 1 and 24.2 kJ mol −1 , respectively, which are much superior to many catalysts previously reported. The high catalytic activity and satisfactory durability endow Ru 0.85 Pd 0.15 /g-C 3 N 4 desirable potential in the hydrogen generation from the hydrolysis of chemical storage materials.

研究领域: 材料科学 · 化学工程 · 能源科学
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NANOTECHNOLOGY · 2018 ·Vol. 29 ·期 46 ·465401 · IF 3.404

Graphitic carbon nitride as polysulfide anchor and barrier for improved lithium–sulfur batteries

Chengxing Li,Kun Gao,Zhipan Zhang

The poor conductivity of sulfur and the shuttle effect of soluble polysulfides have considerably hindered the practical application of lithium–sulfur (Li–S) batteries. Here, we have fabricated a three-dimensional graphitic carbon nitride/reduced graphene oxide (GCN@rGO) network as the sulfur host in Li–S batteries, where the bifunctional GCN strongly binds polysulfides through a chemical interaction and catalyzes the redox reactions of polysulfides. Additionally, GCN coating is also applied to different membranes and when these GCN-coated-membranes (GCMs) are used as separators, they are found to effectively act as the polysulfide barrier to suppress the diffusion of polysulfide intermediates to the Li anode and thus ameliorate the shuttle effect. As a result, the Li–S battery assembled from the GCN@rGO/S cathode and GCM separator exhibited a high initial specific capacity of 1000.6 mAh g−1 at 0.1 C and 87% capacity retention with 0.066% decay per cycle over 200 charge−discharge cycles at 0.5 C.

研究领域: 材料科学 · 电化学
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING · 2014 · IF 1.761

Visible-light enhancement of methylene blue photodegradation by graphitic carbon nitride-titania composites

Dongying Fu,Gaoyi Han,Feifei Liu,Yaoming Xiao,Hongfei Wang,Ruiqin Liu,Cuixian Liu

Composites of graphite-like C 3 N 4 (g-C 3 N 4 ) and TiO 2 were synthesized by direct heating of melamine in the presence of different TiO 2 amounts in a semi-closed stainless steel container. The resulting samples were characterized using X-ray diffraction, X-ray photoelectron spectroscopy (XPS), UV-visible diffuse reflectance spectroscopy (DRS), photoluminescence spectrum (PLS), thermogravimetric analysis , scanning electron microscopy, and transmission electron microscopy techniques. The results reveal that the microstructure and DRS and PLS characteristics of the composites vary with the composition. XPS Ti 2p peaks for the composites exhibit a shift to lower binding energy in comparison to pure TiO 2 . The photocatalytic degradation properties of the composites were evaluated using methylene blue (MB) as a model compound under visible light irradiation (400–600   nm). The results indicate that photocatalytic degradation of MB is higher for g-C 3 N 4 –TiO 2 composites with optimum TiO 2 content (26.4 and 80.0   wt%) than for pure g-C 3 N 4 or TiO 2 . Moreover, the activity of an optimum composite sample was still as high as 91% after use in four consecutive photocatalytic cycles.

CAS / MDL: 108-78-1
研究领域: 材料科学 · 环境科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2021 · IF 19.503

Anchoring strategy for highly active copper nanoclusters in hydrogenation of renewable biomass-derived compounds

Fujun Lan,Jolyon Aarons,Yu Shu,Xiaomei Zhou,Hui Jiao,Hongqian Wang,Qingxin Guan,Wei Li

The hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) is a common reaction that is critical to biomass transformation. However, it is a great challenge to employ non-noble metal catalysts in realizing highly effective conversion from LA to GVL. Herein, we report an efficient strategy for anchoring highly active copper nanocluster catalysts on the defect sites of graphitic carbon nitride (g-C 3 N 4 ) and dispersing in mesoporous silica (SBA-15). The combination of g-C 3 N 4 and SBA-15 stabilized the copper clusters, leading to a high GVL yield of 92 % and excellent stability in 100 h. This result is comparable to that of the Ru/AC catalyst but much more economically favorable. Density functional theory calculations revealed that the reaction barrier of the new catalyst was reduced from 1.93 to 1.12 eV compared with those of unconfined copper particles. This research provides a simple anchoring strategy for constructing highly active and inexpensive copper nanocluster catalysts.

研究领域: 化学工程 · 材料科学 · 催化化学
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JOURNAL OF MEMBRANE SCIENCE · 2021 · IF 8.742

Preparation and decontamination performance of a flexible self-standing hydrogel photocatalytic membrane

Mengyang Lu,Hanmin Zhang

The membrane immobilization of photocatalyst is a kind of win-win mode which can not only avoid the loss of catalyst but also give the membrane antibacterial and self-cleaning properties. Nevertheless, the inefficiency and low durability remain two major obstacles to hinder its practical applications. Herein, a facile micro-solvent combustion synthesis (MSCS) and sodium alginate (SA) crosslinking method were proposed to fabricate an integrated and self-standing membrane of nano-ZnCeOx combined with porous graphitic carbon nitride (ZnCe@PCNM). In the photocatalytic-membrane separation system, the water flux of ZnCe@PCNM was 800 l m −2 •h −1 •bar −1 . Remarkably, the separation efficiency of ZnCe@PCNM could reach more than 90% during the 4-h continuous membrane separation process. The water flux of ZnCe@PCNM under visible light decreased only 21% which was less than that in the absence of light (53%), and the original flux could be completely restored after photocatalysis , signifying that the prepared ZnCe@PCNM had good self-cleaning ability in membrane separation . Meanwhile, ZnCe@PCNM exhibited 99% removal efficiency and 0.06131 min −1 reaction rate in photocatalysis experiments under 1-h visible light. The removal efficiency of ZnCe@PCNM was 1.2-fold and 2.8-fold that of carbon nitride particles (CN) and hydrogel membrane morphology (CNM), respectively. The optical properties test of ZnCe@PCNM showed that its excellent photocatalytic activity was derived from the rapid electron transfer caused by cross-linked structure, heterojunction and the oxygen vacancies induced by nano-ZnCeOx. The radical quenching experiment and EPR experiment showed that •O 2 − and •OH both were the main factors in reaction.

研究领域: 环境科学 · 材料科学
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BIOSENSORS & BIOELECTRONICS · 2014 · IF 6.451

A signal “on” photoelectrochemical biosensor for assay of protein kinase activity and its inhibitor based on graphite-like carbon nitride, Phos-tag and alkaline phosphatase

Huanshun Yin,Bing Sun,Linfeng Dong,Bingchen Li,Yunlei Zhou,Shiyun Ai

A highly sensitive and selective photoelectrochemical (PEC) biosensor is fabricated for the detection of protein kinase activity based on visible-light active graphite-like carbon nitride (g-C 3 N 4 ) and the specific recognition utility of Phos-tag for protein kinase A (PKA)-induced phosphopeptides . For assembling the substrate peptides, g-C 3 N 4 and gold nanoparticles (g-C 3 N 4 -AuNPs) complex is synthesized and characterized. When the immobilized peptides on g-C 3 N 4 –AuNPs modified ITO electrode are phosphorylated under PKA catalysis, they can be specifically identified and binded with biotin functionalized Phos-tag (Phos-tag–biotin) in the presence of Zn 2+ . Then, through the specific interaction between biotin and avidin , avidin functionalized alkaline phosphatase (avidin-ALP) is further assembled to catalyze its substrate of l -ascorbic acid-2-phosphate trisodium salt (AAP) to produce electron donor of ascorbic acid (AA), resulting an increased photocurrent compared with the absence of phosphorylation event. Based on the specific identification effect of Phos-tag, the fabricated biosensor presents excellent selectivity for capturing the phosphorylated serine residues in the substrate peptides. With the good photoactivity of g-C 3 N 4 and ALP-catalyzed signal amplification , the fabricated biosensor presents high sensitivity and low detection limit (0.015   unit/mL, S / N =3) for PKA. The applicability of this PEC biosensor is further testified by the evaluation of PKA inhibition by HA-1077 with the IC 50 value of 1.18   μM. This new strategy is also successfully applied to detect the change of PKA activity in cancer cell lysate with and without drug stimulation. Therefore, the developed PEC method has great potential in screening of kinase inhibitors and highly sensitive detection of kinase activity.

研究领域: 生物化学 · 分析化学 · 医学检测
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POLYMERS FOR ADVANCED TECHNOLOGIES · 2019 ·Vol. 30 ·期 9 ·2458-2467 · IF 2.162

Metal-organic framework MIL-53 (Fe)@C/graphite carbon nitride hybrids with enhanced thermal stability, flame retardancy, and smoke suppression for unsaturated polyester resin

Zhongwei Chen,Tingting Chen,Yuan Yu,Qingwu Zhang,Zhiquan Chen,Juncheng Jiang

Metal-organic framework MIL-53 (Fe)@C/graphite carbon nitride hybrid (MFeCN), a novel flame retardant, was synthesized by hydrothermal reaction and subsequently added into unsaturated polyester resin (UPR). The structure, morphology, and thermal stability of MFeCN were characterized by Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy-dispersive X-ray spectroscopy (EDS), and thermogravimetric analysis (TG). The thermal stability and flammability of the UPR composites were characterized by TG and cone calorimeter tests (CCT). The results of CCT demonstrated that the peak heat release rate (pHRR), total heat release (THR), peak smoke production rate (pSPR), and total smoke production (TSP) of UPR/MFeCN-4 were reduced by 39.8%, 10.2%, 33.3%, and 14.5%, respectively, comparing with UPR. The results of TG and CCT indicated that MFeCN could improve the thermal stability, flame retardancy, and smoke suppression properties of the UPR composites. The residues after CCT were then characterized by laser Raman spectroscopy (LRS), XPS, and SEM. Finally, based on the above experimental results and analysis, the flame retardancy mechanism of MFeCN was proposed.

研究领域: 材料科学 · 化学工程
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