NANOTECHNOLOGY
·
2024
·Vol. 35
·期 49
·495704
·
IF 2.9
Gang Xiao,Zishuai Wang,Yu Jin,Fengping Wang
The selective cleavage of lignin C–C bonds is a highly sought-after process with the goal of obtaining low-molecular-weight aromatic chemicals from renewable resources. However, it remains a challenging task to achieve under mild conditions. Photocatalysis is a potentially promising approach to address this issue, but the development of efficient photocatalysts is still in progress. In this study, we introduce the heterostructured TiO2@g-C3N4 photocatalyst for the development of a visible light photocatalytic procedure for the selective cleavage of lignin C–C bonds under mild conditions. The photocatalyst displays favourable visible light absorption, efficient charge separation efficiency, and promising reusability. A typical β–O–4 dimer model, 2-phenoxy-1-phenylethanol, was effectively (96.0% conversion) and selectively (95.0 selectivity) cleaved under visible light at ambient conditions. This photocatalytic procedure was also effective when subjected to solar irradiation or other lignin dimer models with β–O–4 or β-1 linkages. This reaction occurred through a Cβ-centred radical intermediate and a six-membered transition state with photogenerated holes as the primary active species. The Cα–OH oxidative dehydrogenation of the substrate could also take place but was a relatively minor route. This study provides a new photocatalytic procedure for visible-light-driven lignin valorisation and sheds light on the design of high-performance nanocomposite photocatalysts for C–C bond cleavage.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Eryu Wang,Yi-Chun Chu,Wenjun Zhang,Yanping Wei,Chuanling Si,Regina Palkovits,Xin-Ping Wu,Zupeng Chen
The co-production of hydrogen and value-added biochemicals from lignocellulose utilizing solar energy has been regarded as one of the technologies most potentially able to alleviate the current energy crisis. Here, we demonstrate a cost-effective photoreforming strategy for lignocellulose valorization using a carbon nitride-supported platinum single-atom photocatalyst. An advanced H 2 evolution rate of 6.34 mmol mol Pt –1 h –1 is achieved over the optimal catalyst, which is around 4.6 and 30.5 times higher compared with the nanosized Pt counterpart and pristine carbon nitride, respectively. Meanwhile, the monosaccharides are oxidized to value-added lactic acid with >99% conversion and extraordinary selectivity up to 97%. The theoretical calculations show that with Pt incorporation, the photogenerated holes are predominantly localized on the metal sites while the photogenerated electrons are concentrated on C 3 N 4 , thus enhancing the effective separation of charge carriers. This work provides a promising avenue for the simultaneous production of green H 2 and bio-based chemicals by biomass photorefinery.
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CHEMICAL PHYSICS LETTERS
·
2025
·
IF 3.1
Kangyue Qiao,Songyao Du,Yue Wang,Tongxin Xiao,Guodong Hao,Chao Sui,Yihan Yan
To address the severe Cr(VI) contamination in industrial wastewater, an NH 2 -MIL-101(Fe)/g-C 3 N 4 type-II heterojunction photocatalyst was synthesized via a solvothermal one-pot method. Structural characterization using XRD, SEM, XPS, and BET confirmed successful composite formation with high specific surface area and favorable interfacial contact. Photocatalytic experiments revealed that under conditions of pH = 2, a catalyst dosage of 20 mg, and an initial concentration of 10 mg/L, NM-101(Fe)/0.2CN achieved a 99.5 % reduction efficiency within 80 min. Its reaction rate constant was 3.6 times higher than that of NM-101(Fe) used alone. This study provides new insights for developing highly efficient MOF/polymer composite photocatalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yang Wan,Jiejing Liu,Huijie Wang,Xianghai Song,Weiqiang Zhou,Xin Liu,Jisheng Zhang,Yangyang Yang,Xiaojie Zhang,Binrong Li,Pengwei Huo
The inherent chemical stability of polyethylene terephthalate (PET) poses significant challenges for its natural degradation, leading to severe environmental accumulation. This study presents an innovative Co 1-x S/g-C 3 N 4 S-scheme heterojunction photocatalyst designed to enhance interfacial electron transfer and promote cobalt redox cycling for efficient peroxymonosulfate (PMS) activation, achieving effective PET degradation. Experimental results demonstrated that the optimized photocatalysis/PMS system achieved a 6.3-fold higher PET degradation efficiency compared to the photocatalysis system alone. The optimized system (30 % Co 1-x S/g-C 3 N 4 with 4 mM PMS and 1 mL H 2 O 2 under irradiation) achieved a remarkable PET degradation efficiency of 80.91 ± 1.30 %. Density functional theory (DFT) calculations unveiled the interfacial electronic structure of Co 1-x S/g-C 3 N 4 , demonstrating hole accumulation on g-C 3 N 4 and electron localization on Co 1-x S. Systematic comparative experiments confirmed the cooperative roles of heterojunction architecture, electron transfer dynamics, cobalt active sites, and H 2 O 2 in PMS activation. Degradation intermediates were identified by gas chromatography spectrometry (GC) and liquid chromatography-mass spectrometry (LC-MS), while electron spin resonance (ESR) and radical trapping experiments established SO 4 •− as the predominant reactive species. This study provides a new approach for the construction of S-scheme heterojunction photocatalysts, the activation by PMS, and the treatment of PET plastic in water.
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MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 6
·1-11
·
IF 5.3
Zhang Hui,Ji Yahui,You Nana,Hu Xiaoping,Chen Feifei,Wang Fei,Liu Gen
Ratiometric electrochemiluminescence (ECL) assays have attracted widespread attention in biosensing owing to their precise measurements by eliminating environmental interferences. In this work, g-C 3 N 4 , gold nanoparticles, CuO and luminol were integrated onto hollow carbon spheres (HCS) in sequence to fabricate potential-resolved ECL nanoprobes. The system consists of g-C 3 N 4 as cathode ECL emitters and luminol as anode ECL emitters. The ECL of g-C 3 N 4 is quenched by CuO due to the resonance energy transfer (RET). However, after adding dopamine (DA), the ECL signal is restored due to the redox reaction between CuO and DA. Meanwhile, there is a quenching effect between DA and luminol because DA interferes with the radical reaction process of luminol. Therefore, DA causes the reciprocal changes in cathodic ECL and anodic ECL. This phenomenon can be leveraged to create a ratiometric ECL signal, enabling the quantitative detection of DA. The developed ECL sensor exhibited a sensitive detection toward DA, performing a wide linearity in the range 5.0 × 10 –4 ~ 1.0 × 10 –9 M with a low detection limit of 2.3 × 10 –11 M (S/N = 3). Furthermore, this strategy exhibited a good practicality to detect DA in human urine, providing a promising strategy in ECL bioanalysis. Graphical abstract
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Nanomaterials
·
2025
·Vol. 15
·期 14
·1131
·
IF 4.3
Xing Wei,Gaopeng Jia,Ru Chen,Yalong Zhang
In this study, the BPTCD/g-C3N4heterojunction photocatalyst was successfully prepared by the hydrothermal method. BPTCD (3,3′,4,4′-benzophenone tetracarboxylic dianhydride) is immobilised on the surface of g-C3N4by non-covalent π-π stacking. The BPTCD/g-C3N4heterojunction photocatalyst is an all-organic photocatalyst with significantly improved photocatalytic performance compared with g-C3N4. BPTCD/g-C3N4-60% was able to effectively degrade MO solution (10 mg/L) to 99.9% and 82.8% in 60 min under full spectrum and visible light. The TOC measurement results indicate that MO can ultimately be decomposed into H2O and CO2through photocatalytic action. The photodegradation of methyl orange by BPTCD/g-C3N4composite materials under sunlight is mainly attributed to the successful construction of the heterojunction structure and its excellent π-π stacking effect. Superoxide radicals (•O2−) were found to be the main active species, while•OH and h+played a secondary role. The synthesised BPTCD/g-C3N4also showed excellent stability in the activity of photodegradation of MO in wastewater, with the performance remaining above 90% after three cycles. The mechanism of the photocatalytic removal of MO dyes was also investigated by the trap agent experiments. Additionally, BPTCD/g-C3N4-60% demonstrated exceptional photodegradation performance in the degradation of methylene blue (MB). BPTCD/g-C3N4heterojunctions have great potential to degrade organic pollutants in wastewater under solar irradiation conditions.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Xiaoyan Wang,Yu Yuan,Jingru Lai,Xiaoli Shi,Mingye Ding
Solar-driven water splitting for hydrogen production is a pivotal technique for sustainable energy conversion. However, its efficiency is constrained by intermittent solar irradiation and rapid charge recombination. To overcome these limitations, designing a round-the-clock photocatalyst with high charge storage capacity that can still operate effectively under low light flux after sunset and promote charge carrier separation is a promising strategy. Herein, by selecting SrAl 2 O 4 :Eu 2+ /Dy 3+ persistent phosphors as electron-trapped centers and g-C 3 N 4 semiconductor as visible-light photocatalyst, SrAl 2 O 4 :Eu 2+ /Dy 3+ @g-C 3 N 4 composite has been successfully synthesized via in-situ growth strategy to form a conventional type II heterojunction photocatalyst. Benefiting from the excellent ability of charge storage and release from electron traps and the improved electron-hole separation efficiency, the designed round-the-clock photocatalyst exhibits the improved hydrogen production from 153.8 μmol g −1 h −1 to 560 μmol g −1 h −1 under visible-light irradiation, infrared-light-driven H 2 production of 932 μmol g −1 for 3 h and a dark activity of 269.1 μmol g −1 h −1 lasing for 0.5 h. This work provides a promising strategy for designing a highly efficient photocatalyst for wide-spectral-responsive and all-weather photocatalytic hydrogen production.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Mengying Xu,Jingyan Zheng,Pier-Luc Tremblay,Xiangyang Jiang,Chun He,Yujie Wang,Muhammad Babur Joya,Tian Zhang
Amid the pursuit of renewable energy, photocatalytic H 2 evolution (PHE) and biosynthetic processes gained attention. Bulk g-C 3 N 4 (CN) was calcined under the atmosphere and various gases (air, CO 2 , N 2 , and Ar) to achieve ultra-thin nanosheets. Using greenhouse gas CO 2 for the calcination (CN–CO 2 ) results in a greater PHE rate than in the atmosphere and air, similar to inert gases N 2 and Ar. Under visible light, CN–CO 2 produced H 2 2.6 times faster than CN. Therefore, CN–CO 2 was chosen to promote polyhydroxybutyrate (PHB) production by Cupriavidus necator H16 in hybrid photosynthetic system. The heterotrophic PHB production was increased to 9.14 g/L, which was 1.9 times higher than without the photocatalyst (4.93 g/L), and 1.1 times more than with CN (8.11 g/L). The autotrophic PHB production was also enhanced by adding CN–CO 2 . In summary, the dual benefits of PHE and biological stimulation were achieved by calcining g-C 3 N 4 in CO 2 .
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SENSORS AND ACTUATORS B-CHEMICAL
·
2020
·
IF 7.1
Qiaomei Yuan,Lin Li,Yurong Tang,Xinfeng Zhang
In this work, we reported a photocatalytic biosensor for visual detection of superoxide dismutase (SOD) based on Pt-doped graphite phase carbon nitride (g-C 3 N 4 ). Upon illumination by a violet light-emitting diode (LED), Pt-doped g-C 3 N 4 absorbed the light energy and catalytically produced O 2 − which further oxidized the dyes into a colorless end product. In the presence of SOD, it can specifically catalyze O 2 − into oxygen and hydrogen peroxide, leading to a reduced photooxidation and a visual color display. After screening a series of dyes, the azo dye amaranth (AM) was proven to be the best indicator for O 2 − since the azo bond is active and easily oxidized by O 2 − , resulting in a low background. Such a simple photocatalytic sensor allows visual detection of SOD at a nM level without the need of any sophisticated instrument; using spectrometry, the linear response for SOD detection ranges from 1.5 to 4500 nM with a limit of detection (LOD, 3σ) down to 0.3 nM. The sensor was also successfully applied for label-free and wash-free detection of SOD in human serum samples with a satisfactory recovery.
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BIOSENSORS & BIOELECTRONICS
·
2022
·
IF 12.545
Siyu Luo,Fanglei Liu,Siyu Gu,Ke Chen,Guohai Yang,Yingqiu Gu,Juntao Cao,Lu-Lu Qu
Food-borne pathogens are one of the leading causes of food poisoning, which vigorously affect food safety and human health. Therefore, the development of early and rapid detection methods for food pollution evaluation is the key to food safety and quality control. Herein, a simple and inexpensive photoelectrochemical (PEC) sensor is developed for highly selective and ultrasensitive detection of Staphylococcus aureus (S. aureus). The technique is based on “signal-off” that employs Cu–C 3 N 4 –TiO 2 heterostructures as photoactive materials and monolayer Cu–C 3 N 4 nanozyme as a signal amplifier. In the presence of S. aureus , the aptamer-modified Cu–C 3 N 4 (Cu–C 3 N 4 @Apt, a signal amplifier) and S. aureus were specifically anchored on the surface of the ligand-modified photoelectrode . The Cu–C 3 N 4 @Apt nanozyme acted as a peroxidase to catalyze the oxidation of 4-chloro-1-naphthol (4-CN) to produce insoluble precipitate on the electrode surface and resulted in a significant decrease in photocurrent . Based on the signal-amplification by the Cu–C 3 N 4 @Apt nanozyme, the constructed PEC sensor demonstrated a wide linear range between 10–10 8 CFU/mL for the S. aureus detection with the detection limit (LOD) as low as 3.40 CFU/mL. Furthermore, the PEC sensor was capable of determining S. aureus in spiked orange juice and milk, with the recovery of 91%–113%, indicating the reliability of the sensor for S. aureus detection in real samples. This investigation provides a feasible strategy for the design of highly selective and ultrasensitive PEC sensors to determine analytes in complex systems.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Xiaodong Yang,Minghui Li,Zhiyong Hou,Xuefei Yang,Yuanxia Guo,Shuaiqi Luo,Jin Zhao,Kai Wang,Pengkai Sun,Qiang Yang,Rui Chen,Shuo Yang,Xin Lu,Lulu Liu,Lili Wang,Ye Han,Fanming Zeng,Bin Gao
Norfloxacin, a quinolone antibiotic pollutant, posed a significant threat to environment and human being health. In this study, hydrotalcite-based g-C 3 N 4 composites were produced using electrostatic self-assembly and the structural memory effect of hydrotalcite to optimize their adsorption-degradation of norfloxacin under visible-light illumination. Optimized hydrotalcite and g-C 3 N 4 composite (750°C, 40 wt% of g-C 3 N 4 ) exhibited a highest photo-degradation rate constant of 1.8×10 −2 min −1 with 83.98 % norfloxacin degradation achieved within 1.5 h under visible-light, surpassing that of bare g-C 3 N 4 and hydrotalcite photocatalysts. The synergistic effects of the composite, such as uniform flower-like micro-morphology and rich mesoporous structure, resulted in a large specific surface area (58.67 m 2 /g), abundant active sites, and good photo-generated charge separation efficiency. All these facilitated both sorption (7.95 mg/g) and subsequent visible-light degradation of norfloxacin. Furthermore, the superior photocatalytic performance observed in the degradation of norfloxacin under visible-light illumination was assigned to the effective transport of photogenerated electrons and holes between hydrotalcite and g-C 3 N 4 components. The work highlights the potentials of hydrotalcite and g-C 3 N 4 composites as an excellent photocatalyst for environment remediation and water treatment.
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DALTON TRANSACTIONS
·
2019
·Vol. 48
·期 10
·3486-3495
·
IF 4.052
Juying Lei,Bin Chen,Weijia Lv,Liang Zhou,Lingzhi Wang,Yongdi Liu,Jinlong Zhang
A TiO2/g-C3N4 composite photocatalyst with an inverse opal structure and heterojunction has been successfully prepared by a relatively facile approach. The catalyst was characterized by a combination of XRD, SEM, HRTEM, XPS, PL, EIS and DRS techniques and applied for the photocatalytic degradation of organic pollutants represented by Rhodamine B, phenol and levofloxacin. The results of RhB degradation showed that the rate constant of inverse opal TiO2/g-C3N4 with the best compound ratio is 0.184 min−1, which is 2.7 times faster than that of normal TiO2/g-C3N4 and 4.2 times faster than that of inverse opal TiO2. The enhancement of photocatalytic activity may be attributed to the matched overlapping band structure and the interaction between inverse opal g-C3N4 and TiO2. The inverse opal structure of g-C3N4 has improved the optical absorption properties of g-C3N4 and the interaction between inverse opal g-C3N4 and TiO2 creates more interfaces for the efficient transfer of photogenerated electron–hole pairs to restrict the recombination, which was proved from the photoluminescence spectra (PL). Moreover, a possible photocatalytic mechanism has been tentatively proposed according to the experimental results. All in all, both the inverse opal structure and heterojunction construction play significant roles in the excellent photocatalytic degradation performance according to the mechanism investigation.
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