JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Dong Li,Renyi Li,Yizhou Zhao,Kaixuan Wang,Ke Fan,Wei Guo,Qi Chen,Yujing Li
Perovskite CsPbBr 3 quantum dot shows great potential in artificial photosynthesis, attributed to its outstanding optoelectronic properties. Nevertheless, its photocatalytic activity is hindered by insufficient catalytic active sites and severe charge recombination. In this work, a CsPbBr 3 @Ag-C 3 N 4 ternary heterojunction photocatalyst is designed and synthesized for high-efficiency CO 2 reduction. The CsPbBr 3 quantum dots and Ag nanoparticles are chemically anchored on the surface of g-C 3 N 4 sheets, forming an electron transfer tunnel from CsPbBr 3 quantum dots to Ag nanoparticles via g-C 3 N 4 sheets. The resulting CsPbBr 3 @Ag-C 3 N 4 ternary photocatalyst, with spatial separation of photogenerated carriers, achieves a remarkable conversion rate of 19.49 μmol·g −1 ·h −1 with almost 100 % CO selectivity, a 3.13-fold enhancement in photocatalytic activity as compared to CsPbBr 3 quantum dots. Density functional theory calculations reveal the rapid CO 2 adsorption/activation and the decreased free energy (0.66 eV) of *COOH formation at the interface of Ag nanoparticles and g-C 3 N 4 in contrast to the g-C 3 N 4 , leading to the excellent photocatalytic activity, while the thermodynamically favored CO desorption contributes to the high CO selectivity. This work presents an innovative strategy of constructing perovskite-based photocatalyst by modulating catalyst structure and offers profound insights for efficient CO 2 conversion.
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ACS Applied Materials & Interfaces
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2024
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IF 8.3
Yana Xiao,Zihua Li,Bingang Xu
Flexible and stretchable triboelectric nanogenerators (TENGs) have been rapidly advanced owing to the demand for portable and wearable electronic devices that can work under universal or motional circumstances. While versatile materials can be applied in a TENG as dielectric materials, flexible and cost-effective electrodes are crucially important for the output performance of TENGs. Herein, we developed a poly(vinyl alcohol) (PVA) hydrogel TENG doped with a novel two-dimensional material, graphitic carbon nitride (g-C3N4), which could act as both a cost-effective flexible electrode and a positive dielectric for TENG with different morphologies. The measured peak-to-peak open-circuit voltage of the TENG reached 80 V at a dopant concentration of 2.7 wt % in single-electrode mode, which is far higher than that of the pristine PVA hydrogel TENG. As a demonstration of the application, the g-C3N4/PVA hydrogel TENG can be adopted as electronic skin to monitor the movement of the human body. Low-frequency mechanical energy-harvesting devices in different morphologies including discoid flake shape, tube shape, and spiral shape in the single-electrode mode or contact-separation mode have been designed, fabricated, and evaluated. All of these merits of the proposed hydrogel TENG after doping two-dimensional (2D) material g-C3N4 have demonstrated their promising potential for versatile applications in biomechanical energy harvesting and self-powered sensing.
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WATER RESEARCH
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2024
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IF 11.4
Xueli Hu,Zhi Zhang,Peng Lu,Yuanhang Zhou,Yingying Zhou,Yun Bai,Juanjuan Yao
Without light at night, the system for photocatalytic degradation of refractory organic pollutants in aquatic environments based on free radicals will fall into a dormant state. Hence, a round-the-clock photocatalyst (CCN@SMSED) was prepared by in situ growth of cyanide-deficient g-C 3 N 4 on the surface of Sr 2 MgSi 2 O 7 :Eu 2+ ,Dy 3+ through a simple calcination method. The CCN@SMSED exhibits an outstanding oxidative degradation ability for refractory tetracycline (TC) in water under both light and dark conditions, which is attributed to the synergistic effect of free radical (•O 2 − and •OH) and non-radical (h + and 1 O 2 ). Electrochemical analyses further indicate that direct electron transfer (DET) is also one of the reasons for the efficient degradation of TC. Remarkably, the continuous working time of the round-the-clock photocatalyst in a dark environment was estimated for the first time (about 2.5 h in this system). The degradation pathways of TC mainly include demethylation, ring opening, deamination and dehydration, and the growth of Staphylococcus aureus shows that the process is biosafe. More importantly, CCN@SMSED holds significant promise for practical application due to its low energy consumption and suitability for removing TC from a variety of complex water bodies. This work provides an energy consumption reference for the practical application of round-the-clock photocatalytic degradation of organic pollutants.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Yihao Zhao,Bingzhu Wang,Qimin Fang,Songyang Wu,Yuan Ma,Changxiang Xie,Haiwang Wang
To achieve efficient photocatalytic degradation of multi-component wastewater, the solvothermal method was employed to synthesize g-C 3 N 4 /BiOBr, leading to a homogeneous encapsulation of lamellar g-C 3 N 4 around the flower-like spherical BiOBr structure. In this work, the control of the temperature and the composition ratio during the solvothermal process was used to achieve the modulation of the g-C 3 N 4 /BiOBr microscopic morphology and enhance the photocatalytic activity, and the mechanism of the evolution of its microstructure and photocatalytic activity was elucidated. Moreover, the electron transport bridge between heterojunctions was constructed by introducing metal Pd, which further reduced the probability of photogenerated electron-hole complexation, leading to a higher photocatalytic performance. The elimination rates of RhB, Cr(VI), and TCH of g-C 3 N 4 /Pd/BiOBr under the irradiation of visible light were 99.74 %, 89.20 %, and 44.62 %, respectively, which achieved efficient elimination of a wide range of pollutants. Besides, the carrier transport mechanism in g-C 3 N 4 /Pd/BiOBr heterojunction was proven to Z scheme, which mainly induced the complexation of e - in the conduction band of BiOBr and h + in the valence band of g-C 3 N 4 , which provided higher energy for oxidation and reductive degradation. This work provides an important reference for the research focusing on photocatalyst design and sewage treatment.
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LANGMUIR
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2024
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IF 3.7
Linlin Huang,Xuwen Zhang,Tingting Liu,Lin Wang,Lixin Li,Da Li,Tao Sheng,Zilong Dong,Xinyue Zhao
A coal tar pitch-based porous carbon adsorbent (CPA) was synthesized through a straightforward method involving the heating of a mixture of KOH and coal tar pitch (CTP). This CPA exhibited a high surface area of 1811.2 m2 g–1 and a large pore volume of 0.94 cm3 g–1 when prepared with a CTP to KOH mass ratio of 1:4 at 800 °C. Parameters such as the heating temperature and activator dose were optimized to enhance the adsorption efficiency. The prepared CPA was extensively characterized by SEM, XRD, FTIR, and BET measurements. Notably, CPA presented a distinct adsorption performance for Orange G (OG), achieving a maximum adsorption capability of 449.7 mg g–1. Kinetic studies indicated that the adsorption process followed the pseudo-second-order model, while the adsorption isotherm data demonstrated that both chemical and physical interactions favored OG adsorption. Thermodynamic analysis revealed that the adsorption of OG on CPA was spontaneous and exothermic and increased the entropy. Density functional theory (DFT) calculations provided insights into the adsorption mechanism, highlighting electrostatic interactions, hydrogen bonds, and π–π interactions as the dominant processes governing OG adsorption onto the adsorbent.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Hongji Chen,Yan Wu,Huiping Xiao,Hongfei Yin,Qian Fei,Chunyu Yuan,Qiuyu Zhao,Yujin Zhang,Yongzheng Zhang,Woonming Lau
Owing to the low conversion efficiency of Fe 3+ to Fe 2+ during the peroxymonosulfate (PMS) activation process, the design of an efficient Fenton-like catalyst is still a challenge. In this work, 0D/2D Co-doped Fe 2 O 3 /g-C 3 N 4 (CNCFO) composite catalysts were constructed for organic pollutant degradation, where the Co-doping not only boosts the conversion efficiency of Fe 3+ to Fe 2+ , but also acts as active site for PMS activation. Among them, CNCFO2 showed excellent catalytic performance, where 96.4% of MO could be degraded within 45 s. X-ray photoelectron spectroscopy (XPS) confirmed that the cobalt doping promoted the cycle of Fe 3+ /Fe 2+ , which was responsible for the enhanced PMS activation. Meanwhile, the good stability and reusability of CNCFO2 itself provide opportunities for its potential practical applications. Based on systematical characterizations, the Z-scheme photo-Fenton mechanism was proposed. This study offers a fresh perspective on the advancement of designing highly efficient Fenton-like catalyst for applications in the field of environmental purification.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Chuanhao Li,Yi Tian,Shuangyu Wang,Ping Yang,Xiao Zhang
To improve the stability of Ag based co-catalysts and to increase the photocatalytic performance of graphitic carbon nitride (g-C 3 N 4 ), Ag 2 Se nanoparticles were grown onto superior thin sulfur-doped g-C 3 N 4 nanosheets which was fabricated via two-step thermal polymerization at high temperature. Ultrathin S-doped g-C 3 N 4 nanosheets were prepared via two-step thermal polymerization using melamine and thiourea. The ratios of Ag 2 Se were adjusted to fabricate a series of Ag 2 Se/S-g-C 3 N 4 (Ag 2 Se/SCN) composite samples by controlled solvothermal synthesis. S-doping plays an important role in mono-dispersion of Ag 2 Se nanoparticles on S-g-C 3 N 4 nanosheets because of the control of growth sites. The photocatalytic removal of tetracycline hydrochloride test indicates that sample Ag 2 Se/SCN-3 with Ag 2 Se loading of 3 % reveals the best removal effect, in which tetracycline hydrochloride of 60 % is removed within 60 min. Photocatalytic hydrogen generation test results without co-catalyst addition demonstrate that sample Ag 2 Se/SCN-3 exhibits the best H 2 evolution rate of 2116.35 μmol·g −1 ·h −1 , which is 3.8 times of that of pure carbon nitride. The photocatalytic mechanism tests suggest that Schottky heterojunctions are formed in the Ag 2 Se/S-g-C 3 N 4 composites. The formation of Schottky heterojunctions improved the separation efficiency of photogenerated charge carriers. The incorporation of Ag 2 Se nanoparticles (as the co-catalyst) on S-g-C 3 N 4 nanosheets is the key for drastically improving the photocatalytic performance and eliminating the use of Pt co-catalyst during the photocatalytic processes.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2024
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IF 4.1
Yu Zhang,Mengfei Tian,Bin Qiao,Jiabo Cheng,Yaru Zhang,Kuiwang Chen,Jie Liu,Chunjian Zhao,Chunying Li
As one of the most widely used antibiotics, sulfamethoxazole (SDZ) poses significant health risks to the ecological environment by causing harm to aquatic organisms and accelerating evolution of antibiotic resistant bacteria. Metalloporphyrin hydrogen-bonded organic framework (PFC-72) demonstrates promising prospect in the field of photocatalysis owing to its high specific surface area, wide light harvesting range, stable physical and chemical properties, and semiconductor properties. Herein, we constructed an efficient photocatalyst PFC-72/g-C 3 N 4 by one-step solvent thermal method for photocatalytic degradation of SDZ. When doping content of PFC-72 is 10 %, photocatalytic degradation efficiency of SDZ can reach 96.82 % after 120 min of visible light irradiation, and PFC-72/g-C 3 N 4 exhibits excellent structural stability. The photocatalytic efficiency of SDZ is improved by increasing specific surface area, enhancing absorption range of visible light, and inhibiting recombination of photogenerated electron-hole pairs. In addition, photodegradation pathways of SDZ in PFC-72/g-C 3 N 4 was determined by UPLC-MS/MS analysis. Finally, dominant reactive species (·O 2 − , h VB + , and ·OH) in the system were detected through free radical masking experiments, and photocatalytic mechanism was clarified. This work investigates a novel and efficient porphyrin-HOF based photocatalyst, which has great potential for degradation of SDZ.
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Surfaces and Interfaces
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2024
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IF 5.7
Qian Cheng,Xiaohan Liu,Chuhan Huang,Hongman Sun,Fazle Subhan,Xinyi Zhou,Yuankai Liu,JiaHui Yang,Qi Li,Youhe Wang,Zifeng Yan
Recently, there has been a growing interest in the fundamental understanding of the mechanism of how MIL-101(Fe)/g-C 3 N 4 heterojunctions facilitate the occurrence of photocatalytic nitrogen fixation reactions, especially the electron transfer mechanism has attained increasing attention in photocatalysis. Herein, we implemented a "triple win scenario" strategy to fabricate the S-scheme MIL-101(Fe)/g-C 3 N 4 heterojunction through a straightforward solvothermal process. The MC-6 heterojunction minimizes the recombination of photogenerated carriers, enhances light utilization efficiency, and activates the N≡N bond, thus boosting photocatalytic nitrogen fixation efficiency. The transition metal iron activates the N≡N bond, while S-scheme heterojunctions reduce the photogenerated carrier recombination. In addition, the decrease in band gap (E g ) leads to an increase in visible light utilization efficiency. ISIXPS proved the mechanism of interelectron transfer of MIL-101(Fe)/g-C 3 N 4 heterojunction under illumination. Upon the creation of the heterojunction, electrons migrate from g-C 3 N 4 to MIL-101(Fe), establishing an inherent electric field due to the disparate Fermi levels between the two materials. The electrons (e - ) on the g-C 3 N 4 CB with a more negative reduction potential and the holes ( h + ) on the MIL-101(Fe) VB are retained, which increased the redox capacity to a great extent required for the reduction of N 2 to NH 3 . The ammonia production efficiency of MC-6 photocatalyst was 160 µmol g cat -1 h -1 , representing an 8-fold and 2.8-fold improvement over pristine g-C 3 N 4 (20 µmol g cat -1 h -1 ) and MIL-101(Fe) (57 µmol g cat -1 h -1 ), respectively.
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TALANTA
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2019
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IF 4.916
Menghan Zang,Huijuan Su,Lihua Lu,Feng Li
A group of luminescent dinuclear Ir(III) complexes were synthesized to study the application possibility as luminescent G-quadruplex (G4) sensors. According to the results, the dinuclear Ir(III) complexes 1 – 5 were assessed as selective G4 sensors. Among them, complex 5 not only demonstrates the highest specificity towards G4, but also shows linearly enhanced luminescent intensity with the increase of split G4 concentration. Complex 5 was thus utilized to establish a label-free split G4-based detection platform for luminescent detection of transcription factor (TF). This luminescent assay is simple and sensitive with the detection limit of 0.027 nM for NF-κB p50 in aqueous solution. The split G4-based TF sensing platform also worked well in diluted human serum, demonstrating high application potential for biological sample analysis.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Cheng Chen,Lei Chen,Xiaoying Zhu,Baoliang Chen
Low water flux and heavy membrane fouling hinder the use of graphene-based membranes for water purification and molecular sieving. To the end, a novel graphene-based membrane, intercalated with Ag nanoparticles anchored g-C 3 N 4 (AgNP@g-C 3 N 4 ) as pillars and photocatalysts, was fabricated through a mixed-dimensional assembly strategy. The uniform loading of Ag nanoparticles on g-C 3 N 4 can greatly improve the photocatalytic ability of g-C 3 N 4 while creating more water transport channels between reduced graphene oxide (rGO) and g-C 3 N 4 laminates. The resultant rGO/AgNP@g-C 3 N 4 nanofiltration membrane displayed efficient water permeability, superior photocatalytic self-cleaning performance, and owned excellent flexibility and structural stability. The water permeability of the rGO/AgNP@g-C 3 N 4 membrane was considerably improved (210.9 L∙m −2 ∙h −1 ∙bar −1 ) compared to the pure rGO membrane (78.4 L∙m −2 ∙h −1 ∙bar −1 ) due to the larger interlayer spacing and rough surface. After 1 h of visible light irradiation, the decrease of flux produced by pollutant molecule adsorption can recover with a ultrahigh flux recovery ratio (FRR) of 98.1%. Moreover, the high flux of the rGO/AgNP@g-C 3 N 4 membrane remained stable in a cross-flow photocatalytic nanofiltration device. Membrane separation, photocatalytic regeneration, and pollutant degradation by ·OH and ·O 2 − radicals are proposed as effective cooperation mechanisms.
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PHYSICA B-CONDENSED MATTER
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2024
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IF 2.8
Yongyi Li,Huixing Yang,Wei Li,Zhigang Shao,Yongzhuo Yu,Huixiang Yan,Shichao Jiao,Di Lin,Wenxu Zhang,Chaoyu Lv,Yuxin Huang
In this work, ultrathin lamellar g-C 3 N 4 /In 2 S 3 S-scheme heterojunctions doped with P were synthesized by urea recrystallization and investigated to see which ratio was more favorable for photocatalysis. The P doping formed a new Fermi energy level and reduced the forbidden bandwidth. The ultrathin lamellar structure facilitated rapid charge transfer, and the formation of S-scheme heterojunction, the presence of the interfacial electric field, and band bending effectively separated strong redox-capable electron-hole pairs, thus significantly improving the photocatalytic performance. Among the prepared materials, the 50UP-C 3 N 4 /In 2 S 3 photocatalyst with 50 % UP-C 3 N 4 mass fraction showed optimal photocatalytic H 2 production performance, with a hydrogen production rate of 12,387 μmol h −1 g −1 . Moreover, it showed good performance in photocatalytic degradation, with a degradation efficiency of up to 90.2 % of ofloxacin after 120 min of light exposure. This article provided a new perspective on the synthesis of other photocatalysts with carbazide-based S-scheme heterojunction structures.
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