ULTRASONICS SONOCHEMISTRY
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2022
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IF 9.336
Jiabei Wang,Zhiqiang Jiang
A series of porous S-doped carbon nitride ribbons (PSCN) were prepared by one-pot hydrothermal and sonochemical synthesis techniques. The morphologies and nanostructures of the catalysts were characterized by SEM, XRD and IR, which confirmed the pristine graphitic structures of carbon nitrides retained in the products. Due to sonication treatment, PSCN has porous structures in the thin ribbon and larger specific surface areas (PSCN 43.5 m 2 /g, SCN 26.6 m 2 /g and GCN 6.5 m 2 /g). XPS and elemental mappings verified that sulfur atoms were successfully introduced into the carbon nitride framework. Diffuse reflectance spectroscopy (DRS) results showed S-doping in the carbon nitride reduced the bandgap energy and enhanced their capability of the utilization of visible light, which contributed to higher photo-generated current. Photoluminescence (PL) analysis indicates the recombination of photogenerated carriers was suppressed in PSCN. Moreover, the photocatalytic performance showed that S-doping and porous and thin ribbon nanostructures may effectively boost the CO 2 reduction rate (to as much as 5.8 times of GCN) when illuminated by visible light (>420 nm) without the need of sacrificial materials. The preliminary mechanisms of the formation of PSCN and its applications in photocatalytic CO 2 reduction are proposed. It highlights the potential of the current technique to produce effective, nonmetal-doped carbon nitride photocatalysts.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
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2023
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IF 4.7
Junchang Liu,Minghui Zhu,Weijie Yuan,Guoying Yang,Chen Zhang,Huayang Zhang,Dafeng Zhang,Peiqing Cai,Xipeng Pu
A unique lamellar WO 3 /AgI S-scheme heterojunction is constructed via integrated hydrothermal and coprecipitation methods. Optimized WO 3 /AgI composite shows significantly enhanced photocatalytic ciprofloxacin (CIP) degradation under visible light irradiation, achieving a removal rate of 53.4 % within 3 h, which is about 7.63 and 1.56 times superior than those of pristine WO 3 and AgI, respectively. The characterizations, experiment results and Density Functional Theoretical (DFT) calculation results confirm the enhanced light absorption, well-aligned straddling band structures and reasonable formation of S-scheme heterojunction with efficient photogenerated carriers transfer between WO 3 and AgI. Moreover, O 2 − and h + are identified as the main active species, with O 2 − plays a dominant role in WO 3 /AgI during the photocatalytic degradation of CIP. This work elucidates a possible approach to develop photocatalysts with a high antibiotic removal efficiency through a higher reducing ability and stronger oxidizing ability of S-scheme heterojunction by reasonable structure configuration.
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NANOTECHNOLOGY
·
2023
·Vol. 34
·期 39
·395503
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IF 3.5
Zhiwen Li,Zhilin Zhou,Jianghua Wang,Tingxian Tao,Yingqiang Fu
Carbon quantum dots (CQDs) have been extensively researched as fluorescent probes, but there are few reports on fluorescence-enhanced probes. Herein, nitrogen and sulfur co-doped CQDs (N, S-CQDs) with blue aggregation-induced emission enhancement (AIEE) fluorescence were synthesized by a one-step hydrothermal reaction. N, S-CQDs can rely on the presence of –OH, C=O, –NH2, and ether bonds on their surfaces and the formation of hydrogen bonds by ciprofloxacin (CIP) containing Ar-F and –COOH functional groups to achieve effective charge transfer. In addition, CIP forces N, S-CQDs to aggregate to form cross-linked structures, which effectively limits the vibration and rotation of N, S-CQDs, leading to enhanced fluorescence of N, S-CQDs. Based on the above intermolecular charge transfer and AIEE between N, S-CQDs and CIP, an efficient and sensitive nano fluorescent probe for the detection of CIP in real water samples was developed, which can achieve sensitive detection of 3.33 × 10−8–1.13 × 10−6 M CIP.
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CHINESE JOURNAL OF CATALYSIS
·
2023
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IF 16.5
Zhihan Yu,Chen Guan,Xiaoyang Yue,Quanjun Xiang
Enhancing the carrier separation in graphitized carbon nitride (g-C 3 N 4 ) is advantageous for improving its photocatalytic activity. Herein, we propose a feasible method for preparing CN-C by thermal polymerization to gradually infiltrate carbon rings (C-rings) into the surface of crystalline carbon nitride (CN), enabling photogenerated electrons to be transferred rapidly between the CN inner layers and the CN/C outer layer. Successful penetration and distribution of carbon rings into carbon nitride were confirmed by secondary ion mass spectroscopy using ratio analysis of C and N elements at various depths of the prepared photocatalyst. Theoretical calculations indicated that CN and CN/C in the molecule generated different Fermi levels to form an S-scheme homojunction, establishing appropriate built-in electric fields and thus enabling interlayer charge migration. Moreover, the overlap of the conjugate plane of C-rings with carbon nitride led to the formation of photogenerated in-plane charge transfer tunnels. The two-electron transfer tunnels greatly improved the dissociation efficiency of photogenerated electrons. The prepared sample loaded with 3 wt% Pt as a co-catalyst for hydrogen production under visible light irradiation, and the prepared optimal sample CN-C showed a maximum quantum efficiency of 15.56% for photocatalytic H 2 evolution at 385 nm. This research introduces a new idea for constructing a directional transfer path for charge carriers in-plane and intralayer.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Donghong Duan,Kaixin Chen,Chongzhi Xing,Xiaoqiang Wang,Xianxian Zhou,Shibin Liu
The development of lithium-sulfur (Li-S) batteries necessitates the creation of efficient cathode materials . By simultaneous phosphating and sulfurating, a spindle-shaped CoP-Co 3 S 4 heterostructure sulfur cathode substrate made up of numerous tiny needle-like structures is created. The benefits of CoP with outstanding conductivity and Co 3 S 4 with great adsorption capacity are combined in the as-prepared CoP-Co 3 S 4 heterostructures, which achieve efficient capture-diffusion-transformation of polysulfides at the interface. The CoP accelerates the redox kinetics toward polysulfide conversion, and the Co 3 S 4 has a considerable adsorption power toward polysulfides. The quick nucleation of polysulfide and increased capture effectiveness are aided by the quick transfer of polysulfide from the Co 3 S 4 surface to the CoP surface. As a result, the CoP-Co 3 S 4 @S cathode battery with a 1.1 mg cm −2 sulfur load achieves a high initial capacity of 1516.9 mAh g −1 at 0.2 C and maintains that capacity after 100 cycles at 750.1 mAh g −1 . After 300 cycles, even the 565.1 mAh g −1 specific capacity can be attained at 1 C.
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ACS Applied Materials & Interfaces
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2023
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IF 9.5
Hailin Pan,Jie Wang,Zhi Chen,Ziqi Su,Zheng Tang,Zaifei Ma
Developing transparent conductors to replace indium tin oxide (ITO) is a critical objective in the field of organic optoelectronics. Non-atomically doped (NAD) ZnO thin films, while currently exhibiting limited conductivity, are highly promising candidates due to their unique advantages, such as having complete transparency in both the visible and near-infrared spectral regions, solution processability, and the desired surface electronic properties. In this work, the impact of surface modification by insulating polymers on the ultraviolet-enhanced conductivity of NAD-ZnO films is investigated. It was found that polymer modifiers that are rich in amino and hydroxyl groups are effective at increasing the concentration of oxygen vacancies and the conductivity of NAD-ZnO films. The highest conductivity of over 1000 S cm–1, which is more than twice as high as the previous record for NAD-ZnO films, is achieved using polyethylenimine ethoxylated (PEIE) to modify NAD-ZnO films. Subsequently, the replacement of ITO in organic photovoltaic devices by a ZnO/PEIE electrode is realized. The ZnO/PEIE-based OPV devices that were created exhibit performances comparable to those of ITO-based devices under simulated solar illumination and performances better than those achieved with ITO-based devices under simulated indoor illumination. These results make NAD-ZnO a promising candidate for the widespread replacement of ITO in optoelectronic devices.
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Materials Today Communications
·
2023
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IF 3.8
Yuan Li,Huigui Zhang,Wenyao Qian,Yong Xia,Dongmei Li,Zhiqiang Guo
In recent years, the emerging S-scheme heterojunction photocatalyst has embodied great potential in promoting the research and application of photocatalytic technology. Herein, a new TiO 2 /g-C 3 N 4 S-scheme heterojunction photocatalyst (TCN-20) was constructed by decorating graphite-like carbon nitride on sea urchin-like TiO 2 microspheres with a large specific surface area and a mesoporous structure. TCN-20 has excellent optical absorption ability, effective photogenerated electron-hole pair separation and very high photocatalytic degradation activity in the simulated sunlight. The degradation rate of TCN-20 for Rhodamine B reaches 96.5 %, and the reaction rate constant is 4.98 and 4.52 times higher than that of pure TiO 2 and g-C 3 N 4 , respectively. Moreover, X-ray photoelectron spectra, Fermi level and band structure analyses as well as radical quenching experiments authenticate the S-scheme charge transfer mechanism of TCN-20. TCN-20 is an easy-to-prepare, non-toxic, inexpensive and promising S-scheme heterojunction photocatalyst with strong redox ability.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 30
·期 6
·16156-16165
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IF 5.19
Hou Guangying,Huang Zaihui,Ding Xiaohu,Liu Chunguang
4,4′-Sulfonyl-diphenol (BPS), as a widespread environmental hormone-like micropollutant, is difficult to be degraded in the environment. In this study, the removal of BPS with multi-enzymes extracted from waste sludge and reed sediment was studied at 298 K, 310 K, and 328 K. Results show that BPS could be removed efficiently and was time–temperature dependent, which could involve enzymolysis and bio-flocculation. The mechanism and pathways of the enzymolysis were identified with ultraperformance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS). Polymerization of BPS with enzymolysis further improved the removal by bio-flocculation due to the production of BPS oligomers. Furthermore, the interaction mechanism between BPS and multi-enzyme was explored through a series of spectroscopic experiments. Results show that more loose skeletal structure of the multi-enzymes and more hydrophobic microenvironment of the amino acid residues are responsible for the removal of BPS. This research not only provided a method for refractory micropollutants removal but also a way for the utilization of waste sludge and reed sediment.
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高影响因子
APPLIED CATALYSIS A-GENERAL
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2022
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IF 5.723
Chaofeng Chang,Yuhua Xie,Fang Luo,Shaowei Zhou,Zehui Yang
To economically realize proton electrolyte membrane water splitting technology, stable and high-performance oxygen evolution reaction (OER) electrocatalyst is significantly demanded. In this work, we invite tungsten atoms to metallic iridium (Ir) to weaken s-d hybridization of Ir-Ir bond due to the higher electronegativity accepting electron from Ir atoms; as a result, the adsorbed O* species become electrophilic favorable for the nucleophilic attack by H 2 O leading to 22 % decrement in energy barrier for the formation of OOH* species. Therefore, iridium-tungsten (IrW) electrocatalyst exhibits 3.7-fold higher turnover frequency (TOF) than metallic Ir at overpotential of 370 mV in acidic OER catalysis. Moreover, stable OER performance is recorded due to the high cohesive energy of tungsten atoms. Additionally, TOF of IrW electrocatalyst reaches 10.1 s −1 at overpotential of 100 mV in acidic hydrogen evolution reaction (HER) test, 7.6-time higher than Pt/C and metallic Ir. IrW electrocatalyst only needs 1.52 V to attain 10 mA cm −2 in acidic overall water splitting.
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JOURNAL OF CATALYSIS
·
2022
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IF 8.047
Feiying Tang,Guangji Zhang,Liqiang Wang,Jianhan Huang,You-Nian Liu
Engineering unsymmetrical coordination is an efficient strategy for improving the performance of carbon supported single-atom catalysts for diverse applications. However, the exploration of this strategy to prepare carbon supported single-atom catalysts for hydrogenation reaction is still in infancy, especially for hydrogenation of quinolines. Herein, we report a protein-metal-ion-network strategy for preparation of single-atom cobalt supported on hierarchically porous carbon (SA-Co/NSPC). SA-Co/NSPC features unsymmetrically N/S-coordinated metal center, i.e., Co 1 –N 3 S 1 . Moreover, the carbon matrices possess an ultra-thin two-dimensional morphology and hierarchically porous structures. SA-Co/NSPC catalyst with Co 1 –N 3 S 1 active site exhibits excellent catalytic performance for hydrogenation of N-heterocycles. The DFT calculation results show that the site of Co 1 –N 3 S 1 reveals a significant electron redistribution in comparison to the Co 1 –N 4 , leading to a lower H* diffusion barrier and quinoline hydrogenation reaction barrier. SA-Co/NSPC catalyst combined with the unique hierarchically porous structure and high active Co 1 –N 3 S 1 owns extraordinary catalytic performance for hydrogenation of quinolines.
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CHEMOSPHERE
·
2022
·
IF 8.943
Yanzhuo Zhang,Jing Zhao
The goal of this work was to elucidate the ability of biochar materials prepared by different methods to degrade antibiotics by activating peroxymonosulfate (PMS). S atom was doped into biochar using diphenyl disulfide (DD), sodium thiosulfate (ST), and thiourea (TU) as S precursors. The different doped materials were used to activate PMS and tested for the ability to degrade tetracycline hydrochloride, sulfadiazine sodium salt, and levofloxacin hydrochloride. The average degradation efficiencies of DD-doped hydrothermal + pyrocarbon (DD-HPBC), TU-doped hydrothermal + pyrocarbon (TU-HPBC), and ST-doped hydrothermal + pyrocarbon (ST-HPBC) were 83.76%, 86.74%, and 93.60%, respectively, all higher than the degradation efficiency of the undoped material. When sodium thiosulfate-doped pyrocarbon (ST-PBC), hydrochar (ST-HBC), and hydrothermal + pyrocarbon (ST-HPBC) were used to activate PMS, the highest degradation efficiencies were achieved, with average rates of 71.59%, 78.22% and 97.20%, respectively. ST-HPBC exhibited the highest concentration of environmentally persistent free radicals (EPFRs), 9.47 × 10 18 spin/g, among all biochar materials. Given this high concentration of EPFRs, use of ST-HPBC to activate PMS resulted in a very high rate of antibiotic degradation, and the concentration of EPFRs was positively correlated with the degradation efficiency. Increase of specific surface area, the thiophene S (-C-S-C-) ratio, and concentration of EPFRs in S-doped biochars promoted the degradation of antibiotics. For PMS activated by biochar, reactive oxygen species (ROS) degraded antibiotics in the order of sulfate radical (SO 4 •- ) > singlet oxygen ( 1 O 2 ) > hydroxyl radical (•OH) > superoxide radical (•O 2 − ). This work provides new insight into the application of S-doped sludge biochar materials.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Tiantian Fu,Lingtao Sun,Guijun Li,Yang Xiang,Yibo Tang,Jingqi Sha,Ying Lei,Zhongping Xiong,Yujun Si,Chaozhong Guo
A nitrogen and sulfur codoped carbon-based catalyst (Fe-NS-AG-C) to oxygen reduction reaction (ORR) is prepared by pyrolyzing a precursor from iron chloride, thiourea, anhydrous glucose and carbon black. Glucose is transformed to carbon sheets with defect-rich structures which are highly active to the anchoring of nitrogen and sulfur atoms. Correspondingly, the 3.35 at% and 0.63 at% contents of nitrogen and sulfur in Fe-NS-AG-C are heavily higher than the 0.71 at% and 0.26 at% in the controlled catalyst Fe-NS-C (without glucose). The edge-oriented pyridinic N is easily formed as ORR active sites with the C-S structure. A dual mesopore-dominated microstructure is also constructed by the carbon sheets to favor the mass transfer in the reaction process. As a result, the Fe-NS-AG-C presents outstanding ORR performance with more positive half wave potential, greater limiting current density, and better methanol tolerance than the benchmark Pt/C catalyst. The Zn-air battery assembled with Fe-NS-AG-C outputs 1.48 V of open circuit voltage, 156 mW cm −2 of maximum power density, and 1.26 V of work voltage, 785 mAh g −1 Zn of specific capacity and 983 mWh g −1 Zn of specific energy density at 10 mA cm −2 of discharge current density.
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