Catalysis Science & Technology
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2021
·Vol. 12
·期 4
·1144-1158
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IF 6.119
Junke Li,Mei Li,Zhiliang Jin
An S-scheme surface heterojunction between Co3S4 and Mo2S3 was constructed successfully via a stepwise hydrothermal method. A rhombic dodecahedral cobalt-based metal–organic zeolite imidazole framework (ZIF-67) is used as the cobalt source and template to participate in the reaction process. ZIF-67 with a dodecahedral structure is first reshaped into cobalt sulfide with a hollow polyhedral structure via a one-step sulfidation reaction. And then, Mo and S species were introduced on the surface of Co3S4 to fabricate Co3S4@Mo2S3 with a hierarchical core–shell structure and S-scheme heterojunction. In comparison, the H2 evolution activity of Co3S4@Mo2S3 is about 7 and 3 times higher than those of pure Mo2S3 and Co3S4. Density functional theory (DFT) calculations were used to construct the molecular model of Co3S4 and Mo2S3, and the sample's energy band structure was also analyzed. Based on the analysis of a series of characterization results, a H2 evolution mechanism of Co3S4@Mo2S3 with a S-scheme surface heterojunction was proposed. The formation of the S-scheme surface heterojunction between Co3S4 and Mo2S3 results in a more developed channel to transfer photogenerated electrons and allows the system to retain a more effective redox potential. Besides, the Mo2S3 nanosheet's criss-cross growth on the Co3S4 surface is beneficial to the improvement of the cycle stability of the Co3S4@Mo2S3 composite. This work uses a ZIF-67 polyhedron as the template to provide a new strategy for preparing a hierarchical S-scheme surface heterojunction photocatalyst based on MOFs.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Lin Liu,Jiaqing Liu,Weijie Yang,Jun Wan,Feng Fu,Danjun Wang
Energy band structures greatly determine the charge separation and transfer properties in heterojunction photocatalysts and consequently their photocatalytic activities. Herein, a well-designed Z-scheme ZnIn 2 S 4 -S/CNTs/RP (ZIS-S/CNTs/RP) nanocomposite was fabricated according to an energy band alignment steering strategy to realize superior photocatalytic H 2 evolution performance. The ZIS-S/CNTs/RP nanocomposite shows an efficient photocatalytic H 2 evolution rate of 1639.9 μmol g -1 h −1 , which is noticeably higher than that of pristine red phosphorus (RP) and CNTs/RP and ZIS-S/RP composites, as well as those of the compared heterojunctions using bulk RP or ZnIn 2 S 4 . Owing to the modification of nanosized RP and the introduction of sulfur vacancies in ZnIn 2 S 4 , a tailored energy band alignment of the heterojunction with a higher reduction potential and larger Fermi level potential difference was achieved, which resulted in significantly increased photogenerated electron-hole separation efficiency and a more efficient Z-scheme charge transfer mechanism, thus promoting the photocatalytic activity of ZIS-S/CNTs/RP. This work aims to provide a novel effective strategy for the construction of high-performance heterojunction photocatalysts by energy band engineering.
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JOURNAL OF MOLECULAR RECOGNITION
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2021
·Vol. 34
·期 11
·e2930
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IF 2.137
Haipeng Ye,Ji Shao,Yanpeng Shi,Siwei Tan,Kewen Su,Ling Zhang,Xiaoyue Shan
In this study, magnetic molecularly imprinted polymers (MMIPs) were prepared and used as sorbents for extraction of S-phenylmercapturic acid (S-PMA) from urine samples, followed by high-performance liquid chromatography ultraviolet-visible (HPLC-UV/Vis) analysis. The MMIPs were synthesized by the copolymerization reaction of (phenylthio) acetic acid (template molecule), methacrylic acid (functional monomers) and ethylene glycol dimethacrylate (cross-linkers). The morphology, structure property and surface groups of the prepared MMIPs were characterized by scan electron microscopy, transmission electron microscopy, infrared spectroscopy, X-ray diffraction pattern, thermogravimetric analyses, Brunauer-Emmett-Teller and vibrating sample magnetometer. The selectivity of the MMIPs was investigated in the presence of interferents. Various parameters affecting the S-PMA extraction efficiency were investigated, including MMIPs amount, pH, sample volume, desorption solvent, as well as extraction and desorption time. The obtained optimal parameters were as follows: MMIPs amount (20 mg), pH (3.0), sample volume (5 mL), desorption solvent (methanol/acetic acid [9/1, v/v]), extraction time (30 minutes) and desorption time (2 minutes). The method was validated according to the Food and Drug Administration Guidance for Industry on Bioanalytical Method Validation. The calibration curve for the analyte was linear in the concentration range of 0.030-1.0 mg/L ( r = 0.9995). The LOD and LOQ of the method were 0.0080 and 0.0267 mg/L, respectively. The enrichment factor of the MMIPs was 5. The relative standard deviations of intra- and inter-day tests were in the range of 3.8-5.1% and 3.9-6.3%, respectively. The recoveries at three different concentrations of 0.10, 0.50 and 0.80 mg/L ranged between 95.2% and 98.6%. In addition, the MMIPs could be reused for at least eight times. The proposed method was successfully applied to the determination of S-PMA in urine samples. In addition, this developed method could be used as a tool in the early screening and clinical diagnosis of benzene intoxication.
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Journal of Cleaner Production
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2021
·
IF 9.297
Yuan-Yuan Yu,Zhong-Qiu Liu,Guo-Qiang Zhang,Yu-Jing Liu,An-Guo Ying
The selective valorization of lignite into monocyclic aromatic compounds (MCACs) is extremely challenging due to its chemical inertness and geometrical complexity. The catalytic efficiency of lignite valorization into MCACs over solid acids is significantly reduced by the presence of H 2 O resulting in the leaching and deactivation of acid sites. Moreover, the precise fabrication of poly(ionic liquid)s (PILs) containing Brønsted-Lewis acidic sites, well-defined mesoporous channels, and hydrophobicity remains a considerable challenge. Herein, a novel hydrophobic mesoporous PILs with strong Brønsted-Lewis acid sites was successfully constructed by a synergistic regulation-induced copolymerization strategy for the first time. More exotically, the resultant multifunctional PILs was found to be ultra-efficient catalyst for the selective valorization of Yiwu lignite (YL) into MCACs with 23.5 wt.% yield, which is the highest yield reported for lignite catalytic valorization by precious metal-free catalysts under mild conditions. The co-catalysis mechanisms of YL valorization into MCACs over the multifunctional PILs are confirmed by characterization methods and the synergistic catalysis mechanisms are as follows: (1) hydrophobic micro-environment: the hydrophobic micro-environment created by hydrophobic block is favorable for preventing the leaching and deactivation of Brønsted-Lewis acid sites; (2) mesoporous confinement: the well-defined mesoporous channels strengthen the adsorption amount of H 2 and increases the concentration of substrates; (3) synergistic catalytic active hydrogen transfer of Brønsted-Lewis acid sites: Brønsted-Lewis acid sites synergistically promote H 2 heterolysis to the mobile H + and immobile H − , and then the resulting mobile H + transfers to oxygen atom in lignite to produce MCACs via C–O bond cleavage . This work not only sheds some light on developing the multifunctional solid acid catalysts , but also demonstrates an efficient catalyzing method to produce lignite-based MCACs by co-catalysis of Brønsted-Lewis acidic sites, mesoporous confinement, and hydrophobic micro-environment.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Qi Xia,Jinlong Hu,Qingqing Chen,Lingzhi Zhang
Selenium cathode attracts great attention due to its high theoretical volumetric capacity and better electrical conductivity than sulfur cathode. Herein, N/S co-doped microporous carbon (NS-K-PC) is designed and prepared as Se host by a spray drying process of the poly(styrenesulfonic acid)-melamine salt solution followed by carbonization and activation process. The as-prepared NS-K-PC shows a very high micropore contribution of 94.8% in the total surface area, and a total N/S heteroatom doping level of 2.5 wt% in the carbon matrix. The NS-K-PC/Se cathode delivers a high reversible capacity of 499.2 mA h g −1 at 0.1C, superior rate capacity of 324 mA h g −1 at 8C, and great cycling stability with a capacity decay of 0.081% per cycle over 500 cycles at 1C. Additionally, a comparative study demonstrates that NS-K-PC/Se cathode with the carbonate-based electrolytes exhibit better cycling stability than those with ether-based electrolytes primarily resulted from a direct solid–solid conversion of Se to Li 2 Se bypassing the formation of soluble polyselenides.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Dongdong He,Ke Zhu,Jin Huang,Yaqian Shen,Lele Lei,Hongmei He,Wenjin Chen
Heteroatoms doped carbon materials are widely used in the advanced oxidation process (AOPs) to remove organic pollutants in water due to the synergies effect between different heteroatoms. In this study, a novel kind of N, S co-doped magnetic mesoporous carbon nanosheets (Fe@NS-C) was prepared by simple one-step pyrolysis . Further, the influence of doping amount of S ( L -methionine) and N (melamine) on catalytic activity was studied, the optimized sample Fe@NS-C-2-12/PMS showed a satisfying degradation ( 91.07%) for high concentrations of tetracycline (80 mg/L TC) in 10 min, which was attributed to the proper ratio of S content to N content (S(at.%)/ N(at.%) = 0.2097) in the sample could better play its synergistic effect by XPS analysis. The Fe@NS-C-2-12/ PMS system also exhibited satisfactory degradation effects in a wide pH range (3−10) and the existence of inorganic ions and humic acid . Then, the degradation mechanisms were mainly through the non-radical pathway ( 1 O 2 and electron transfer) and the major active sites were pyridinic N compared to thiophene S, C O, and Fe-N x . This study could inspire the design of high-performance active and low-cost heteroatomic doping nano-magnetic catalysts for PMS-based waste treatment .
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Liuyun Chen,Xinling Xie,Tongming Su,Hongbing Ji,Zuzeng Qin
Photocatalytic hydrogen production from water splitting production is a promising strategy to solve the energy crisis and environmental pollution. In the present work, Co 3 O 4 /CdS composites were prepared by ultrasonication and stirring, and used for photocatalytic water splitting. The results showed a Co-S chemical bonds were formed at the interfaces between the Co 3 O 4 and the CdS, which promoted the charge transfer rate between the CdS and Co 3 O 4 . Meanwhile, the recombination of the electron-hole pairs was further restrained by the Co 3 O 4 /CdS p-n heterojunction. The 10%-Co 3 O 4 /CdS composites exhibited an excellent photocatalytic hydrogen production rate of 142.62 μmol∙h −1 , which was 20 times higher than that of CdS (6.85 μmol∙h −1 ), and the Co 3 O 4 /CdS showed excellent stability in the photocatalytic water splitting reaction. Moreover, a formation process of Co 3 O 4 /CdS p-n heterojunction and a mechanism of Co 3 O 4 /CdS p-n heterojunction avoiding the recombination of photocatalytic electrons and holes to enhance photocatalytic activity was proposed.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
·
IF 5.316
Shuyun Wan,Xi Liu,Likang Fu,Chengbao Zhou,Hongyi Chen,Guanghui Li,Shiyue Cao,Qiming Liu
Stannous sulfide (SnS) with low-cost and high theoretical specific capacity possesses enormous potential in the application of lithium-ion batteries (LIBs). However, the sluggish Li ion diffusion kinetics and severe volume variation of SnS, result in inferior rate capability and poor cycling stability. Hollow SnS microflower spheres coated with N, S dual-doped carbon (H-SnS@NSC) are constructed through a facile hydrothermal reaction , polydopamine encapsulation and subsequent carbonization process. Such rational hollow structure is conducive to enhance the structural stability of the material. More importantly, N, S dual-doped carbon is synergistically coupled with SnS, which can greatly improve the electrons/ions kinetics and mitigate the volume expansion. As consequence, the H-SnS@NSC composite electrode exhibits an admirable specific capacity of 778.5 mAh g −1 at 0.5 A g −1 after 400 cycles. It still remains a specific capacity of 633.8 mAh g −1 after 800 cycles even at 1.0 A g −1 , corresponding to 81.7% of initial capacity. After being assembled into a full cell, the device delivers a stable capacity of 317 mAh g −1 at 0.1 A g −1 . This work manifests that morphology and structure engineering have bright prospects in promoting the practical applications for metal sulfides.
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CATALYSIS LETTERS
·
2021
·Vol. 151
·期 11
·3170-3188
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IF 3.186
Zhang Qian,Zhou Yu-lian,Wang Bao-zong,Hong Jun-ming
The performance of electrocatalytic-oxidation process depends on the anode characteristics, so the preparation of active anode materials is an attractive method to enhance the efficiency of this process. However, the high catalytic properties of graphene and its derivatives have been well confirmed, an efficient method of controlling catalytic activity and stability remains to be established. In this research, the relationship between the precursor and catalytic performance was clarified by regulating the oxygen-containing groups in the precursor. Results indicated that the surface O groups on the precursor were sensitive to controlling the catalytic activity and stability of tri-doped reduced graphene oxide (RGO). With more O groups in the precursor (catalysts from graphene oxide), the doped heteroatom species is vulnerable involved into reaction, leading to the flaking of active sites, and ultimately decreasing the activity and stability performance. By contrast, the fewer O groups in the precursor (catalysts from RGO) created stable and active defects for oxidation activity. The interactions of O groups in the C precursor with those in the heteroatom precursor were further confirmed by DFT calculations. The findings of this research presented a new strategy for controlling the stability and performance of the resulting catalysts. Graphic Abstract DEME-TFSI-coated GO and GN are first formed via covalent bonds through functional groups (O groups) on the graphene surface, non-covalent ionic bonds, and π–π stacking interactions. In this step, N, S, and F groups are weakly bonded with graphene. Stable pyridine and pyrrole structures could then be generated via dehydration and decarbonylation under a controlled temperature and pressure in the hydrothermal process. Finally, cyclization rearrangement is carried out to form graphite with a tri-doped structure.
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ACS Applied Materials & Interfaces
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2021
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IF 9.229
Kaiqi Wang,Zhenpeng Zhang,Su Li,Haibo Zhang,Nailin Yue,Jinhui Pang,Zhenhua Jiang
To obtain anion exchange membranes with both high ionic conductivity and good dimensional stability, a series of side-chain-type poly(arylene ether sulfone)s (PAES-QDTPM-x) were designed and synthesized. Quaternary ammonium (QA) groups were densely aggregated and grafted onto the main chain via flexible hydrophobic spacers. Well-defined microphase separation was confirmed by small-angle X-ray scattering. PAES-QDTPM-0.30 exhibited reasonably high conductivity (39.4 mS cm–1 at 20 °C and 76.1 mS cm–1 at 80 °C) and excellent dimensional stability at 80 °C (11.9% in length, 11.2% in thickness) due to the concentration of ion clusters and the side-chain-type structure. All membranes maintained over 82% of the conductivity after alkali treatment for 14 days. In the H2/O2 fuel cell performance test, the maximum power density of PAES-QDTPM-0.30 at 60 °C was 225.8 mW cm–2.
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RSC Advances
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2021
·Vol. 11
·期 23
·14193-14202
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IF 3.361
Yang Li,Liguo Wang,Yan Cao,Shuang Xu,Peng He,Huiquan Li,Hui Liu
A series of imidazolinium-based porous poly(ionic liquid)s (PILs) with different anions prepared by free-radical copolymerization of an arene-bridged tris-vinylimidazolium salt and divinylbenzene (DVB) were constructed. The as-prepared PILs were characterized by BET, SEM, TEM, TGA and Elemental Analysis (EA), and the results showed that they had plentiful ionic sites, and abundant and stable mesopores. In particular, the density of ionic sites and pore structure of PILs could be controlled by adjusting the content of DVB. Moreover, the PILs were used as efficient heterogeneous catalysts for the decarboxylation of cyclic carbonates to epoxides for the first time. Results showed that the catalytic activity of PILs was positively correlated with the nucleophilicity of the anions in PILs, and PDVB-[PhTVIM]Cl-1 with a chloride anion-enriched skeleton displayed the best catalytic performance. Without any solvent or cocatalyst, PDVB-[PhTVIM]Cl-1 achieved a TOF value of 108.1 h−1 and the yield of butylene oxide of 89.6%, which was even better than the homogeneous IL-based catalysts (TOF value: 8.7 h−1) that had been previously reported. Meanwhile, PDVB-[PhTVIM]Cl-1 also exhibited excellent recyclability and substrate compatibility.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Shuangyu Wang,Zhiwei Hu,Zhongmou Pan,Dewei Wang
The construction of heteroatom-doped hierarchical carbon frameworks has attracted significant research attention as high-performance electrode materials for supercapacitors. Herein, a facile one-step Mohr’s salt-assisted KOH activation strategy has been developed for the production of S-doped hierarchical carbon frameworks with large specific surface area from sustainable spruce bark. We found Mohr’s salt plays multiple roles during the synthesizing process by simultaneously acting as an S source, the template to generate mesopores, and the co-activator beyond KOH. As the electrode for supercapacitors, the high specific capacitance of 281 and 156 F g −1 can be achieved in aqueous electrolyte and ionic liquid electrolyte at 1 A g −1 , respectively. More importantly, the electrode also displays excellent rate capability where a high capacitance can be maintained at large charge-discharge operation. Moreover, the supercapacitor device also demonstrated an energy density is high up to 66.26 Wh kg −1 at the power density of 875 W kg −1 in ionic liquid electrolyte. These results acquired could offer a versatile way to convert renewable biomass into value-add porous carbon for electrochemical energy-storage applications.
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