APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Peng Wang,Enmin Hu,Linzhen Wu,Junhui He,Yihao Wang,Zhenhong Ou,Fan Yang,Tao Chen,Wenkun Zhu
Photo-assisted uranium extraction from seawater is regarded as a potential technique for uranium resource recovery. Here, we report a polymeric carbon nitride (SCN-C 3 N 4 ) synthesized via a one-step calcination method, which combines cyano groups (-C≡N) modification and S atoms doping for efficient uranium extraction. By DFT calculations, we confirm that the integration of -C≡N modification and S atoms doping effectively reconstructed the charge distribution on the inside of the heptazine rings, forming a strong driving force for the migration of photogenerated electrons to the reactive sites. Accordingly, the reaction rate constant of SCN-C 3 N 4 ( k = 0.00843 min −1 ) is 20.07 times higher than that of g-C 3 N 4 ( k = 0.00042 min −1 ). Finally, the SCN-C 3 N 4 exhibits a remarkable uranium extraction capacity of 6.05 mg g −1 in natural seawater. Relying on various spectroscopic techniques, we identify the reaction process of uranium, which is captured by -C≡N, forming UO 2.34 crystallization under the joint action of electrons and free radicals. Furthermore, SCN-C 3 N 4 demonstrates excellent antibacterial and corrosion resistance, breaking the bottleneck of uranium extraction from marine biofouling. This work provides an example of designing novel polymeric carbon nitride materials for uranium extraction.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Ming-Yang Ma,Min-Yi Chen,Tao Sun,Bin Xue
The wettability of polymeric carbon nitride (PCN) is an important surface chemical factor affecting its catalytic and separation performance. However, due to the amphipathic characteristics of hydrophilic/lipophilic and porous powder properties, the contact angle (CA) of PCN measured by the common sessile drop method will be interfered by the substrate, resulting in randomness of the results. Herein, the pristine PCNs obtained by thermal polycondensation of different precursors in air or nitrogen atmosphere were used as the wettability research object. The CA of the PCNs was measured by a modified sessile drop method after the traditional powders were replaced by pressed-tablet samples. The influence of sample mass and applied pressure on specific surface area, pore volume, surface morphology and CA of the pressed-tablet samples was investigated carefully, and the optimal experimental conditions were determined. When the sample mass was 0.15 g and the applied pressure was 10 MPa, the measured water CA of PCNs was between 27 ∼ 34°, and the diiodomethane CA is between 24 ∼ 29°. The measurement results showed considerable stability and reproducibility. This improved CA measurement method provides a simple and standardized way to accurately explore the surface chemistry of PCN, and has the potential to be applied to other hydrophilic and/or oleophilic porous powder materials.
研究领域:
材料科学
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表面化学
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DOI
高影响因子
Journal of Cleaner Production
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2021
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IF 9.297
Yu Yang,Tao Ji,Yuan Lin,Wenyue Su
Photocatalytic cementitious materials (PCMs) are a promising material for air purification at ambient conditions. Herein, polymeric carbon nitride (PCN), a material with high chemical and thermal stability that is responsive to visible light, was employed for the fabrication of PCMs with the assistance of two adhesives (i.e., acrylic latex and waterglass). The effect of the adhesives on the photocatalytic removal of nitrogen oxides (NO x ) and their stability over the PCN-coated PCMs was studied under various environmental conditions. Experimental results indicated that the waterglass-based PCMs outperformed the acrylic latex-based PCMs in terms of the photocatalytic NO x removal under visible light irradiation and stability in the peeling and washing trials. The relative humidity had beneficial effects on the NO x removal efficiency for the acrylic latex and deleterious effects on the waterglass incorporated PCMs, due to their distinct surface wettability . The ambient temperature, initial nitrogen monoxide (NO) concentration, and light intensity had a positive impact on the NO x removal efficiency for the as-prepared PCMs.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 16
·5663-5670
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IF 6.119
Mengqi Xue,Daochuan Jiang,Haiwei Du,Zhongjun Li,Hong Bi,Yupeng Yuan
Localizing charge carriers close to catalytically active sites can reduce the charge recombination in photoexcited polymeric carbon nitride (PCN), which thus potentially increases its photocatalytic H2 generation. However, this strategy has not been applied to enhance the photocatalytic performance of PCN. Herein density functional theory (DFT) calculations unravel that N defect (Ndefect) engineered tri-s-triazine units form a highly localized mid-gap state in PCN, which can localize the π electrons for efficient separation of electrons and holes. Moreover, Ndefect engineered tri-s-triazine units impart the lowest Gibbs free energy barrier of −0.129 eV for the reduction of H+ to adsorbed H, thereby serving as the catalytically active sites. Enlightened by theoretical results, the Ndefect engineered tri-s-triazine units were created via post oxidation of PCN in an electronic furnace. Such PCN with N defects offers an increased photocatalytic H2 generation under visible light exposure. The highest H2 generation rate is up to 98.1 μmol h−1, 3.8 times higher than that by using pristine PCN (26.1 μmol h−1). This work manifests the significance of localizing charge carriers close to the catalytically active sites for increased photocatalytic performance of PCN.
研究领域:
材料科学
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理论计算化学
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产品关联
DOI
高影响因子
Research
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2021
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IF 0
Yuqing Cheng,Jiafu Shi,Yizhou Wu,Xueying Wang,Yiying Sun,Ziyi Cai,Yu Chen,Zhongyi Jiang
Solar-driven photocatalytic regeneration of cofactors, including reduced nicotinamide adenine dinucleotide (NADH), reduced nicotinamide adenine dinucleotide phosphate (NADPH), and reduced flavin adenine dinucleotide (FADH2), could ensure the sustainable energy supply of enzymatic reactions catalyzed by oxidoreductases for the efficient synthesis of chemicals. However, the elevation of cofactor regeneration efficiency is severely hindered by the inefficient utilization of electrons transferred on the surface of photocatalysts. Inspired by the phenomenon of ferredoxin-NADP+ reductase (FNR) anchoring on thylakoid membrane, herein, a homogeneous catalyst of rhodium (Rh) complex, [Cp∗Rh(bpy)H2O]2+, was anchored on polymeric carbon nitride (PCN) mediated by a tannic acid/polyethyleneimine (TA/PEI) adhesive layer, acquiring PCN@TA/PEI-Rh core@shell photocatalyst. Illuminated by visible light, electrons were excited from the PCN core, then transferred through the TA/PEI shell, and finally captured by the surface-anchored Rh for instant utilization during the regeneration of NADH. The TA/PEI-Rh shell could facilitate the electron transfer from the PCN core and, more importantly, achieved ~1.3-fold elevation of electron utilization efficiency compared with PCN. Accordingly, the PCN@TA/PEI-Rh afforded the NADH regeneration efficiency of 37.8% after 20 min reaction under LED light (405 nm) illumination, over 1.5 times higher than PCN with free Rh. Coupling of the NADH regeneration system with formate dehydrogenase achieved continuous production of formate from carbon dioxide (CO2). Our study may provide a generic and effective strategy to elevate the catalytic efficiency of a photocatalyst through intensifying the electron utilization.
研究领域:
生物化学
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光催化材料科学
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DOI
APPLIED SURFACE SCIENCE
·
2023
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IF 6.7
Feiran Jia,Qing Liu,Liyan Xie,Zhishan Luo,Jianhui Huang,Yingying He,Lirong Qiu
The use of heterojunctions with Z-scheme photocatalysts holds great promise for enhancing the photocatalytic degradation efficiency of antibiotics. In this study, we report the construction of a novel heterostructure by in-situ growth of the ultrathin polymeric carbon nitride (PCN) on the electrospun Bi 2 WO 6 nanofibers for improved photocatalytic tetracycline (TC) degradation under visible light. Our gas–solid reaction strategy enables the formation of uniform and intimate junctions between the PCN nanosheets and the Bi 2 WO 6 nanofibers, resulting in a well-contacted interface that remarkably accelerates the separation and transfer of the photogenerated charge carriers. The optimized PCN/Bi 2 WO 6 photocatalyst exhibits a significant TC degradation rate of 89.5 % under visible light, which is 1.4-fold and 2.0-fold of the pure PCN and Bi 2 WO 6 photocatalysts, respectively. Our innovative design philosophy opens up a new horizon for the development of efficient Z-scheme heterostructured photocatalysts for antibiotic degradation.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Lijun Hu,Yi-Meng Du,Rui Liu,Shisheng Yang,Hongliang Tang,Xue-Zan Yin,Qianxiang Xiao,Xiangke Wang,Hongqing Wang
Photocatalytic hydrogen peroxide (H 2 O 2 ) generation on the catalyst surface from oxygen is an electron-demanding process, making the construction of an electron-rich surface highly advantageous. In this study, a localized electric field was observed on the surface of polymeric carbon nitride (g-C 3 N 4 ) when alkali metal cations were adsorbed onto it. These fields effectively inhibited surface carrier recombination and extended their lifespan, thereby enhancing H 2 O 2 production. As a result, g-C 3 N 4 achieved a superior H 2 O 2 yield of 2.25 mM after 1 h in a 0.25 M K + solution, which was 2.06 times greater than that (1.09 mM) achieved in a pure solvent. Notably, the increase in photocatalytic efficiency showed a remarkable dependence on ion species. At low concentrations, H 2 O 2 generation efficiency was in the order of Li + < Na + < K + < Rb + < Cs + . However, after optimizing the ion concentration, the highest H 2 O 2 production was achieved in a solution containing K + instead of Cs + . Molecular dynamics simulations and temperature-dependent photocatalysis experiments revealed that the synergistic interaction between adsorption energy and adsorption distance was crucial in governing the extent to which alkali metal cation adsorption enhanced g-C 3 N 4 photocatalytic H 2 O 2 production. This study provides theoretical insights for the design of materials for electron-demanding photocatalysis and aids in understanding variations in photocatalytic behavior in natural waters.
研究领域:
材料科学
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环境科学
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化学
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产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
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2021
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IF 8.198
Shuangchao Zhao,Keyan Li,Jun Du,Chunshan Song,Xinwen Guo
The development of high-efficiency photocatalysts is of great importance to realize robust solar-driven CO2 conversion; however, the low carrier separation efficiency and poor light absorption ability usually limit the performance of the photocatalysts. Herein, a hollow In2S3/polymeric carbon nitride (IS/CN) heterojunction was prepared via electrostatic self-assembly and in situ sulfidation under solvothermal conditions. The intimate interfacial contact between the IS and CN facilitates the construction of an effective heterojunction, as demonstrated by X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM). The optimized IS/CN-5 sample exhibits a high CO evolution rate of 483.4 μmol g–1 h–1, which is 99 and 6 times as high as that of IS and CN, respectively. The improved charge separation and transfer efficiency, the hollow nanotube structure, and the enhanced CO2 adsorption ability are the reasons for the excellent photocatalytic activity. Besides, a possible photocatalytic mechanism of CO2 reduction by the IS/CN heterojunction was proposed on the basis of the band structures. This work provides an effective and facile strategy to construct hollow semiconductor heterojunctions for photocatalytic applications.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
APPLIED CLAY SCIENCE
·
2019
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IF 3.89
Xiang Hu,Zhu Shu,Hui Guo,Jun Zhou,Tiantian Li,Yigen Tan,Zihao Liao,Wenbin Wang,Zhengliang Zhao
Nanostructure-tailoring and composite-construction are two effective strategies to optimize polymeric carbon nitride (PCN) for advanced photocatalysis . Herein, a vapor deposition process was adopted to grow PCN nanosheets on the surface of the cheap mineral metakaolin , achieving both the nano-structuring of PCN and the synchronous construction of metakaolin/nano-PCN composite. It showed a substantially improved photocatalytic H 2 evolution activity 3.8 times higher than the traditional bulk PCN under visible light. Performance gains benefit from the natural electronegativity of metakaolin and the nanosizing of PCN, which synergistically facilitate the separation and utilization of photoinduced charge carriers. This work may inspire not only the utilization of various clay minerals but also the nano-tailoring and composite-construction of PCN.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Binrong Li,Na Li,Zhiwei Guo,Chen Wang,Xuedong Wang,Zhi Zhu,Xu Tang,Pengwei Huo
Polymeric carbon nitride (PCN) is an environmentally friendly photocatalyst for solar-driven H 2 O 2 production, but the activity of original PCN is still not satisfactory. The main limitation is the sluggish exciton dissociation leading to slow generation and conversion of superoxide radical (•O 2 − ) intermediate. Herein, the PCN with dual defect sites and compact interlayer is rationally designed for H 2 O 2 photosynthesis with an ultrahigh rate of 3930.9 μmol g −1 h −1 and rapid •O 2 − yield rate of 1.92 min −1 . The enhanced activity is attributed to effective exciton dissociation during interlayer and intralayer process. Moreover, nitrogen vacancies change the oxygen adsorption configuration (formation of C − O − O − C bridge mode), thus promoting O 2 adsorption and activation. A well-matched linear relationship was established between the concentration of nitrogen vacancies and •O 2 − /H 2 O 2 production. This work not only provides in-depth insights for the photocatalytic H 2 O 2 generation mechanism, but also offers a new paradigm for designing efficient PCN-based photocatalysts for energy conversion.
研究领域:
材料科学
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光催化
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能源转换
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Fei Yang,Guiming Ba,Zhen Wang,Haiping Li
Surface modification has been considered a simple and effective strategy to enhance the photocatalytic activity of polymeric carbon nitride (CN), but resultant difference of energy band structures between the modified surface layer and the unmodified inside in the sample has always been neglected. Herein, maleoyl-modified CN (MaCN) was simply prepared via a dehydration reaction between CN and maleic acid, and exhibits enhanced charge separation, optical absorption, and thus photocatalytic hydrogen evolution activity, relative to the bulk CN. The surface modification causes variation of the band structure, suggesting the difference of band levels between the surface layer with maleoyl-modification and the inside without any modification in MaCN, and the surface layer and the inside with matched band levels form type-II core-shell homojunction to enhance the charge separation. This work expounds a conceptual framework of core-shell homojunction in surface-modified CN photocatalysts.
研究领域:
材料科学
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光催化
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化学工程
✓ 已验证
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2019
·Vol. 9
·期 23
·6627-6637
·
IF 5.726
Zhiwei Liang,Yuguo Xia,Guiming Ba,Haiping Li,Quanhua Deng,Wanguo Hou
The high recombination efficiency of photogenerated charge carriers is the primary factor suppressing the photocatalytic performance of polymeric carbon nitride (CN). To enhance the charge separation, Sb-doped CN (CN/Sb) was firstly synthesized using antimonate as a doping and oxidizing agent. The N–SbIII bond was fabricated in CN/Sb via a redox process, which works as a charge-capture center, evidenced by experimental and theoretical calculation methods, and leads to a prominent enhancement in the charge separation and transfer performance of CN/Sb. CN/Sb exhibits much higher photocatalytic activity than CN in water splitting and environmental remediation. The visible-light photocatalytic hydrogen evolution rate of CN/Sb can reach ∼1.75 mmol g−1 h−1, which is ∼4.5 times that of CN, with an apparent quantum yield of 6.4% at 420 nm. Reactive oxygen species generation rates of CN/Sb are also much higher than those of CN. This work provides not only a new effective way for CN modification but also a deep insight into the metal-doping structure in the CN framework, which can guide future research on metal-doped CN photocatalysts.
研究领域:
材料科学
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光催化领域
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）