JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Jinhong Bi,Zhangtong Zhang,Jinjin Tian,Guocheng Huang
Tetracycline (TC) antibiotics, extensively utilized in livestock farming and aquaculture, pose significant environmental challenges. Photocatalysis, leveraging renewable sunlight and reusable photocatalysts, offers a promising avenue for mitigating TC pollution. However, identifying robust photocatalysts remains a formidable challenge. This study introduces a novel hollow-flower-ball-like nanoheterojunction composed of a nitrogen-rich covalent organic framework (N-COF) coupled with BiOBr (BOB), a semiconductor with a higher Fermi level. The synthesized N-COF/BOB S-scheme nanoheterojunction features an expanded contact interface, strengthened chemical bonding, and unique band topologies. The N-COF/BOB composites showcased exceptional TC degradation performance, achieving an 81.2% removal of 60 mg/L TC within 2 h, markedly surpassing the individual efficiencies of N-COF and BOB by factors of 3.80 and 5.96, respectively. Furthermore, the total organic carbon (TOC) removal efficiency highlights a superior mineralization capacity in the N-COF/BOB composite compared to the individual components, N-COF and BOB. The toxicity assessment revealed that the degradation intermediates possess diminished environmental toxicity. This enhanced performance is ascribed to the robust S-scheme nanoheterojunction structure, which promotes efficient photoinduced electron transfer from BOB to N-COF. This process also augments the separation of photogenerated charge carriers, resulting in an increased yield of superoxide radicals (∙O 2 − ) and hydroxyl radicals (∙OH). These reactive species significantly contribute to the degradation and mineralization of TC. Consequently, this study introduces a sustainable approach for addressing emerging antibiotic contaminants, employing COF-based photocatalysts.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Liying Sun,Xuesong He,Bin Liu,Shuming Zhang,Zheng Xiang,Xin Wang,Yang Wang
The development of materials with dual adsorption/photocatalytic functions for the removal of difficult-to-degrade organics is a very promising and challenging strategy. In this paper, a novel S-scheme heterojunction photocatalyst, InVO 4 /ZnIn 2 S 4 , was successfully synthesized with a unique hierarchical structure, which provides plenty of accessible adsorption/photocatalytic sites with a high light-harvesting rate (by multiple reflections). The experimental results show that optimized InVO 4 /ZnIn 2 S 4 (5-IV/ZIS) has superior removal performance, whose adsorption-photocatalytic synergistic removal of tetracycline (TET) can reach 69.31 % after 15 min and 90.69 % after 45 min. Based on the analysis of the mechanism, the excellent removal performance can be attributed to the adsorption of the target onto the material by hydrogen bonding, followed by the degradation of the adsorbed target by active substances ( h + > O 2 •− > e - > 1 O 2 > • OH) generated by the S-scheme heterojunction. In addition, the possible pathways for the photocatalytic removal of TET on 5-IV/ZIS were investigated by HPLC-MS analysis. T.E.S.T. and E. coli inhibition experiments demonstrated a significant reduction in the toxicity of TET after the photocatalytic reaction. In conclusion, the novel multifunctional photocatalyst 5-IV/ZIS prepared in this study can be used for the efficient treatment of organic compounds in wastewater with a bright application prospect.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Bo Wang,Yanhong Liu,Jinhui Hao,Junbo Zhong,Furong Yu,Kewei Zhang,Hao Shen,Baodong Mao
Earth-abundant metal sulfides attracts large attention in recent years for hydrogen production via electrocatalytic water splitting. However, most works have been limited to the acidic condition, whereas the hydrogen evolution reaction (HER) in alkaline condition has rarely been discussed. Here we present an effective strategy for the growing of Co-Mo-S catalysts on carbon cloth via the controllable incorporation of cobalt into MoS 2 with L-cysteine and phosphomolybdic acid to achieve the synergistic interaction of CoS 2 and MoS 2 . The optimized Co-Mo-S catalysts (Co:Mo=1:2) showed a largely improved HER activity with an overpotential of 92 mV at current density of 10 mA cm -2 and Tafel slope of 82 mV dec -1 . The origin of the activity enhancement was investigated through a series of characterizations, where the synergetic effect of the intrinsic fast HER kinetics of metallic CoS 2 and the high active surface area of MoS 2 plays a crucial role. With appropriate amount of cobalt, the Co-Mo-S catalysts show a relatively uniform distribution on the carbon cloth to ensure the large surface area, whereas excessive cobalt results in the formation of the large CoS 2 particles with low HER activity from the low active surface area. Further electrochemical measurements demonstrated that the combination of larger exchange current density of CoS 2 and the high electrochemical double–layer capacitance (proportional to the active surface area) of MoS 2 together contributed to the HER activity enhancement of the Co-Mo-S catalysts. The Co-Mo-S/CC catalysts also show robust stability in alkaline solution. Our work provides a more profound understanding and an interesting view for the design of efficient ternary transition metal sulfide HER catalysts in alkaline condition by synergetic optimization of the intrinsic HER kinetics and the electrochemical active surface area.
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International Journal of Minerals Metallurgy and Materials
·
2022
·Vol. 29
·期 5
·1120-1131
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IF 3.85
Yan Wenjing,Zhang Jintao,Lü Aijing,Lu Songle,Zhong Yiwei,Wang Mingyong
Stable non-noble metal bifunctional electrocatalysts are one of the challenges to the fluctuating overall water splitting driven by renewable energy. Herein, a novel self-supporting hierarchically porous Ni x Fe—S/NiFe 2 O 4 heterostructure as bifunctional electrocatalyst was constructed based on porous Ni—Fe electrodeposition on three-dimensional (3D) carbon fiber cloth, in situ oxidation, and chemical sulfuration. Results showed that the Ni x Fe—S/NiFe 2 O 4 heterostructure with a large specific surface area exhibits good bifunctional activity and stability for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) because of the abundance of active sites, synergistic effect of the heterostructure, superhydrophilic surface, and stable, self-supporting structure. The results further confirmed that the Ni x Fe—S phase in the heterostructure is transformed into metal oxides/hydroxides and Ni 3 S 2 during OER. Compared with the commercial 20wt% Pt/C∥IrO 2 —Ta 2 O 5 electrolyzer, the self-supporting Ni 1/5 Fe—S/NiFe 2 O 4 ∥Ni 1/2 Fe—S/NiFe 2 O 4 electrolyzer exhibits better stability and lower cell voltage in the fluctuating current density range of 10–500 mA/cm 2 . Particularly, the cell voltage of Ni 1/5 Fe—S/NiFe 2 O 4 ∥Ni 1/2 Fe—S/NiFe 2 O 4 is only approximately 3.91 V at an industrial current density of 500 mA/cm 2 , which is lower than that of the 20wt% Pt/C∥IrO 2 —Ta 2 O 5 electrolyzer (i.e., approximately 4.79 V). This work provides a promising strategy to develop excellent bifunctional electrocatalysts for fluctuating overall water splitting.
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Solar RRL
·
2023
·Vol. 7
·期 24
·2300838
·
IF 7.9
Ding Ma,Mengge Li,Bin Yao,Yongfeng Li,Zhanhui Ding,Jiayong Zhang,Chunkai Wang,Yuting Sun,Yue Liu,Xiaofei Sun,Yan Zhu
It is known that high carrier recombination at the p–n junction interface and low carrier separation ability (CSA) are two main problems resulting in low power conversion efficiency (PCE) of the Cu 2 ZnSn(S,Se) 4 (CZTSSe) solar cell. To resolve these problems, one CZTSSe solar cell is prepared through substituting B-doped CdS for CdS in a solar cell with the conventional structure of Ag/ITO/ZnO/CdS/CZTSSe/Mo/SLG and annealing B-doped CdS/CZTSSe/Mo/SLG prior to deposition of ZnO, ITO, and Ag electrode. By optimizing the B doping content in the CdS and annealing temperature and time of the B-doped CdS/CZTSSe, lattice mismatch between CdS and CZTSSe is decreased and width of depletion region is increased, leading to reduction in interfacial recombination, enhancement in CSA and intensity of incident light passing through the B-doped CdS, and so increase in PCE from 7.89% of CZTSSe solar cell using CdS as buffer layer to 10.62%. A mechanism of the increment of the PCE induced by B doping and annealing is suggested. This work proposes a method of increasing PCE of CZTSSe solar cell and advances a deeper understanding of the mechanisms behind various parameters in CZTSSe solar cells through theoretical analysis and calculations.
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APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Qingrui Peng,Haijun Wang,Yongmei Xia,Xiang Liu
A multifunctional Zr-containing catalyst (FM-Zr-ARS) was successfully synthesized by a modulated hydrothermal synthesis route. Systematic characterization results supported the presence of robust porous inorganic-organic frameworks stabilized by the strong coordination interaction of Zr 4+ with oxygen-rich functional groups in Alizarin red S (ARS). Moreover, the -O-Zr-O- network in the FM-Zr-ARS structure formed a rich content of acid-base sites. In addition, the inherent sulfonic groups in ARS made the FM-Zr-ARS hybrids possess Brønsted acid sites. Therefore, under the synergistic catalysis of the multiple functional sites, FM-Zr-ARS showed remarkably high catalytic activity for γ-valerolactone (GVL) production from levulinate esters and furfural. Finally, 72.4 % and 97.7 % yields of GVL were obtained in the conversion of furfural and ethyl levulinate, respectively, after 8 h of reaction at 433 K. On the basis of the role of different functional sites, a plausible catalytic mechanism was presented for the conversion of biomass-derived furfural to GVL.
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CHEMISTRY OF MATERIALS
·
2020
·
IF 9.567
Huanhuan Jia,Xinmiao Liang,Tao An,Linfeng Peng,Jiwen Feng,Jia Xie
Finding sodium solid electrolytes (SSEs) with good performance is key to building all-solid-state sodium batteries. In the development of solid electrolytes, halogen doping has been shown to be an effective approach. However, it has rarely been applied to chalcogenide-based SSEs, possibly because of strict structure constraints. In this work, the strategy of halogen doping is successfully demonstrated on Na3.67[Sn0.67Si0.33]0.67P0.33S4, a novel SSE with high structural tolerance. The halogen-doped samples formulated as Na3.57[Sn0.67Si0.33]0.67P0.33S3.9X0.1 (X = Cl, Br, and I) exhibit higher ionic conductivities and lower activation energies than the pristine sample. Na3.57[Sn0.67Si0.33]0.67P0.33S3.9I0.1, the I-doped sample, has the highest ambient ionic conductivity of 1.08 mS cm–1 and the lowest activation energy of 0.24 eV. Structure analysis indicates that the high electronegativity of Cl atoms plays an important role in improving the conduction of Na+ ions in Cl-doped samples. The large atomic radius and high polarizability of I are more important factors to accelerate the transportation of Na+ ions in the I-doped counterpart. Furthermore, the all-solid-state sodium batteries assembled with Na3.57[Sn0.67Si0.33]0.67P0.33S3.9I0.1 as solid electrolytes show decent cyclic stability at 30 °C with a current density of 0.15 A g–1. This work systematically manifests the effect of halogen doping in SSEs, providing a versatile method to develop novel SSEs.
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Nanomaterials
·
2021
·Vol. 11
·期 10
·2562
·
IF 5.076
Shuang Lian,Yu Wang,Haifeng Ji,Xiaojie Zhang,Jingjing Shi,Yi Feng,Xiongwei Qu
The development of solid-state polymer electrolytes is an effective way to overcome the notorious shuttle effect of polysulfides in traditional liquid lithium sulfur batteries. In this paper, cationic cyclopropenium based cross-linked polymer was firstly prepared with the one pot method, and then the counter ion was replaced by TFSI−anion using simple ion replacement. Cationic cyclopropenium hyper-crosslinked polymer (HP) was introduced into a polyethylene oxide (PEO) matrix with the solution casting method to prepare a composite polymer electrolyte membrane. By adding HP@TFSI to the PEO-based electrolyte, the mechanical and electrochemical properties of the solid-state lithium-sulfur batteries were significantly improved. The PEO-20%HP@TFSI electrolyte shows the highest Li+ionic conductivity at 60 °C (4.0 × 10−4S·cm−1) and the highest mechanical strength. In the PEO matrix, uniform distribution of HP@TFSI inhibits crystallization and weakens the interaction between each PEO chain. Compared with pure PEO/LiTFSI electrolyte, the PEO-20%HP@TFSI electrolyte shows lower interface resistance and higher interface stability with lithium anode. The lithium sulfur battery based on the PEO-20%HP@TFSI electrolyte shows excellent electrochemical performance, high Coulombic efficiency and high cycle stability. After 500 cycles, the capacity of the lithium-sulfur battery based on PEO-20%HP@TFSI electrolytes keeps approximately 410 mAh·g−1at 1 C, the Coulomb efficiency is close to 100%, and the cycle capacity decay rate is 0.082%.
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International Journal of Extreme Manufacturing
·
2022
·Vol. 5
·期 1
·015502
·
IF 10.036
Zhibin Jiang,Lujie Jin,Xiying Jian,Jinxia Huang,Hongshuai Wang,Binhong Wu,Kang Wang,Ling Chen,Youyong Li,Xiang Liu,Weishan Li
Lithium-sulfur (Li-S) batteries can provide far higher energy density than currently commercialized lithium ion batteries, but challenges remain before it they are used in practice. One of the challenges is the shuttle effect that originates from soluble intermediates, like lithium polysulfides. To address this issue, we report a novel laminar composite, N,O-carboxymethyl chitosan-reduced graphene oxide (CC-rGO), which is manufactured via the self-assembly of CC onto GO and subsequent reduction of GO under an extreme condition of 1 Pa and −50 °C. The synthesized laminar CC-rGO composite is mixed with acetylene black (AB) and coated on a commercial polypropylene (PP) membrane, resulting in a separator (CC-rGO/AB/PP) that can not only completely suppress the polysulfides penetration, but also can accelerate the lithium ion transportation, providing a Li-S battery with excellent cyclic stability and rate capability. As confirmed by theoretic simulations, this unique feature of CC-rGO is attributed to its strong repulsive interaction to polysulfide anions and its benefit for fast lithium ion transportation through the paths paved by the heteroatoms in CC.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
FuYin Lan,HaiYan Zhang,Jinchen Fan,Qunjie Xu,Hexing Li,YuLin Min
Herein, we introduce polymer nanofibers of TiO2@NiCo-LDH as interlayers into Li–S batteries. From 0 to 60 °C, the interlayers can deliver high sulfur utilization, an outstanding rate capability, and excellent cycling life. High-temperature excitation makes it easier for the valence band electrons of TiO2 to transition to the conduction band. The electron–hole pairs formed on the surface combine with the ether group of 1,3-dioxolane in the electrolyte, which greatly reduces the decomposition and volatilization rates of the electrolyte, ensuring Li–S batteries with good cycle performance at high temperatures. The capacity can stabilize at 798.6 mAh g–1 after 100 cycles at 60 °C and 1C, and the battery can provide a capacity higher than 323.2 mAh g–1 at 0 °C. Simultaneously, the lithium metal symmetrical battery with a functional separator can be continuously cycled for 1800 and 750 h without a short circuit at the current densities of 0.65 and 1.63 mA cm–2, respectively.
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ACTA PHYSICO-CHIMICA SINICA
·
2023
·
IF 10.9
Kexin Dong,Chuqi Shen,Ruyu Yan,Yanping Liu,Chunqiang Zhuang,Shijie Li
The escalating presence of pharmaceutical antibiotics in natural water poses an overwhelming threat to the sustainable development of society. Photocatalysis technology stands out as a promising and cutting-edge environmental purification alternative. C 3 N 5 , identified as a distinctive nonprecious nonmetal photocatalyst, holds potential for environmental protection. However, challenges persist originating from the sluggish photoreaction kinetics and severe photo-carrier reunion. Currently, the design of a special S-scheme photosystem proves to be a reliable strategy for obtaining outstanding photocatalysts. In this context, a plasmonic S-scheme photosystem involving Ag/Ag 3 PO 4 /C 3 N 5 was developed through a feasible route. The compactly connected 0D/0D/2D Ag/Ag 3 PO 4 /C 3 N 5 heterostructure, benefitting from the synergy between the plasmonic effect and the S-scheme junction, facilitates the efficient utilization of appreciably reinforced sunlight absorption, effective photo-carrier disassociation, and notable photoredox capacity. Consequently, this system generates •OH and
⋅ O 2 - effectively. Ag/Ag 3 PO 4 /C 3 N 5 demonstrates a superb photocatalytic levofloxacin eradication rate of 0.0362 min −1 , marking a substantial advancement of 24.8, 1.1, and 0.7 folds compared to C 3 N 5 , Ag 3 PO 4 , and Ag 3 PO 4 /C 3 N 5 , respectively. Impressively, Ag/Ag 3 PO 4 /C 3 N 5 delivers remarkable anti-interference performance and reusability. This achievement signifies a significant step toward developing potent C 3 N 5 -involved photosystems for environmental purification. Download: Download high-res image (106KB) Download: Download full-size image
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
·
IF 11.2
Shengqian Liang,Min Ma,Zheng Zheng,Jiahang Song,Yijian Zhou,Enzhou Liu,Haixia Ma,Bing Wang,Bo Zhou,Yan Nie,Zhuo Li
For the efficient harnessing of solar energy and mitigation of environmental pollution, the development and application of semiconductor photocatalysis technology is paramount. Herein, a novel SubPc-Br/CdS supramolecular array with an S-scheme heterojunction was synthesized through the intermolecular π-stacked self-assembly of subphthalocyanine (SubPc-Br) and nanometer cadmium sulfide (CdS). This self-assembly system features a highly structured architecture and excellent stability. Experiments and ground-state differential charge calculations demonstrate that SubPc-Br and CdS form a built-in electric field during the self-assembly process, a critical factor in promoting the dissociation of electrons and holes. Additionally, this study utilized time-dependent density functional theory (TDDFT) to simulate the dynamic adsorption behavior of excited oxygen molecules on the SubPc-Br/CdS interface for the first time. The analysis of molecular charge differential density under different excited states proved that the addition of SubPc-Br molecules not only improves the photocorrosion resistance of CdS in an O 2 adsorption environment but also enhances the production of advanced reactive oxygen species under the synergistic action of h + and ·O 2 – . When subjected to visible light, the degradation efficiency of minocycline (MC) achieved 96.8 % within 60 min and maintained 80.3 % after 5 cycles. In summary, this study highlights the feasibility of creating advanced S-scheme heterojunction photocatalysts through the strategic incorporation of organic supramolecules with semiconductor catalysts.
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