CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Yueping Bao,Wen-Da Oh,Teik-Thye Lim,Rong Wang,Richard David Webster,Xiao Hu
A novel Co 3 O 4 nanocatalyst functionalized Al 2 O 3 ceramic membrane (CoFCM) with a honeycomb structure was prepared via an optimized surface-nucleated zeolitic imidazolate framework (ZIF-67) growth method. The Co 3 O 4 hollow structure which was confirmed via chemical characterizations (XRD, FTIR, Raman and XPS), was formed on the membrane surface by one-step calcination of ZIF-67 membrane. The CoFCM was characterized by various techniques including the field emission scanning electron microscopy and atomic force microscopy. The results revealed the formation of well-defined Co 3 O 4 layer on the porous Al 2 O 3 ceramic membrane with the thickness of 1.5–2 µm. The growth mechanism of CoFCM was further proposed via XPS and the catalytic activity of CoFCM was investigated for the removal of sulfamethoxazole (SMX) with the addition of Oxone. The membrane performance was examined under a home-made dead-end mode. Results indicated that CoFCM has a rougher surface with an initial membrane resistance of 1.19 × 10 11 m −1 and performs outstanding catalytic activity. The pure water permeability of CoFCM is 3024 L m −2 h −1 bar −1 , which is comparable to that of the pristine ceramic membrane (<10% difference). The SMX removal efficiency achieved to >90% in 90 min with an Oxone addition of 0.1 g L −1 . Meanwhile, the membrane showed excellent durability by retaining >95% of initial flux for at least 3 operational cycles with a low cobalt ion leaching via Oxone-assisted cleaning. Furthermore, the reaction mechanism of Oxone activation by CoFCM was proposed from the results of the electron paramagnetic resonance (EPR) and radical scavenger experiments.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
ACS Applied Energy Materials
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2025
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IF 5.5
Siwei Guo,Jinhong Wu,Haosen Chen,Ding Huan,Huihua Wang,Deyong Wang,Dong Hou,Xianglong Li
Transition metal sulfides exhibit superior oxygen evolution reaction electrocatalytic performance due to their unique electronic structures and significant surface reconstructions. The electronic structure of transition metal sulfides can be effectively regulated via heteroatom doping, vacancy engineering, interface engineering, and structure engineering, and surface reconstructions can also be coordinated via coupling with electron-donating carbon materials. Herein, a facile cation regulation strategy is reported to boost the oxygen evolution reaction (OER) activity of transition metal sulfides by pyrolyzing and sulfurizing the Fe2+- and Ni2+-modified ZIF-67 precursor (FeNi/ZIF-67). Crucially, Fe doping and Ni substitution in the final products are achieved by a simple room-temperature ion-exchange strategy, significantly boosting the OER activity. Meanwhile, conductive porous carbon from the organic ligand improves the mass transfer and active-site accessibility. As anticipated, Fe-doped CoS2 and NiCo2S4 embedded in N-doped porous carbon (NC) on carbon cloth (CoFe1Ni2S@NC/CC) demonstrate excellent hydrophilicity and OER activity, representing a very low overpotential of 175 mV at 20 mA cm–2, fast reaction kinetics (Rct = 0.51 Ω cm–2), and considerable electrocatalytic durability in 1.0 M KOH. This work offers a simple and low-cost cation regulation method for designing efficient cobalt-based sulfide hybrid electrocatalysts for OER, advancing their application in electrochemical water splitting.
研究领域:
材料科学
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电化学
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Huan Gao,Fengqi Han,Shasha Yi,Lu Chen,Deliang Chen
Perovskite oxide (ABO 3 ) is a potential oxygen evolution reaction (OER) electrocatalyst , and its B-site is generally regarded as the active center. However, perovskite oxides suffer from poor conductivity and insufficient active sites due to severe calcination during high-temperature synthesis. To address these issues, we started from a well-demonstrated OER catalyst Ba 0.5 Sr 0.5 Co 0.8 Fe 0.2 O 3-δ (BSCF) and developed an approach to load abundant active sites with the exsolution of CoFe nanoparticles from parent phase BSCF. During this process, ZIF-67 has been used as the carbon source to generate highly conductive network of cobalt-doped carbon and further fabricated as BSCF/ZIF (67) -650 composite. Such hybrid catalyst exhibits an overpotential of 285 mV at current density of 10 mA cm −2 and a minor Tafel slope of 40 mV dec −1 in 1 M KOH alkaline solution. The remarkably enhanced activity is attributed to the increment of active sites, oxygen vacancies and excellent conductivity. Importantly, such OER performance shows excellent stability for 200 h operation.
研究领域:
材料科学
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电化学
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能量存储与转换
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纳米材料
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催化
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DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
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2022
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IF 3.656
Li-hu Qian,Wei-wei Dong,Min-da Xu,Yan-Bo Cao,Xuan Wu,Xiao-jie Song,Yi Ding,Xi Wang
Developing hybrid metal sulfide electrocatalyst with excellent hydrogen evolution reaction (HER) catalytic performance and stability is vital to its commercial applications. Herein, hybrid CuCo 2 S 4 @ MoS 2 catalysts were designed with CuCo 2 S 4 synthesized by using ZIF-67 as a template and externally decorated with MoS 2 . The hybrid catalysts (denoted as C@M-0.5, C@M − 1, C@M − 2) show improved catalytic activity than those of MoS 2 and CuCo 2 S 4 due to large surface area and the interface between nanoflower-like MoS 2 and three-dimensional interconnected lamellar stacked CuCo 2 S 4 , which boost charge transport capability and improve the HER kinetic process. The influences of different ratio of CuCo 2 S 4 to MoS 2 on the electrocatalytic activity are investigated in detail. Specifically, C@M − 1 exhibit the best HER performance with an overpotential of 143 mV@ 10 mA/cm 2 , a Tafel slope of 45.2 mV/dec and satisfactory long-time stability. This work rationally designs hybrid CuCo 2 S 4 @MoS 2 catalyst to preserve the merits of using the ZIF-67 as a template and make use of the synergistic coupling effects between CuCo 2 S 4 and MoS 2 , which can be extended to synthesize other catalysts in different energy conversion fields.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Jia Xie,Yingpeng Yang,Hao Zhang,Saisai Chen,Zhengjun Lv,Yujun Zhou,Junwen Qi,Xiuyun Sun,Jiansheng Li
Advanced oxidation processes (AOPs) were appealing wastewater treatment options yet practices were hampered by reactor design and diminished performance in complex water matrices. Herein, one-step-pyrolysis strategy was proposed for large-scale synthesis of ZIF-67 derived conductive Co/N carbon hollow fiber ultrafiltration membrane to achieve exceptional availability of catalytic sites and interference prevention from macro molecular substances by size exclusion. Benefitting from the microenvironment modulation and electric field assistance (−1 V, membrane as the cathode), the bisphenol A (as a model micropollutant) can be efficiently removed with enhanced mass transfer of flow-through process (modified apparent reaction rate constant of 1260 μM g cat -1 s −1 ) and the active cobalt species were cycled via electroreduction thus showing exceptional sustainability with nearly zero Co leaching even after 24 h operation. The synergy effects between separation and catalysis alleviated the deteriorated AOPs efficiency and membrane fouling caused by macromolecular organic matter. The integrated membrane system provides new insight into rational design of catalytic membrane and system engineering for advanced water purification.
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Nanomaterials
·
2022
·Vol. 12
·期 9
·1571
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IF 5.719
Hao Gong,Shiguang Bie,Jian Zhang,Xianbin Ke,Xiaoxing Wang,Jianquan Liang,Nian Wu,Qichang Zhang,Chuanxian Luo,Yanmin Jia
The Co3O4electrode is a very promising material owing to its ultrahigh capacitance. Nevertheless, the electrochemical performance of Co3O4-based supercapacitors is practically confined by the limited active sites and poor conductivity of Co3O4. Herein, we provide a facile synthetic strategy of tightly anchoring Co3O4nanosheets to a carbon fiber conductive cloth (Co3O4@C) using the zeolitic imidazolate framework-67 (ZIF-67) sacrificial template via in situ impregnation and the pyrolysis method. Benefiting from the enhancement of conductivity and the increase in active sites, the binder-free porous Co3O4@C supercapacitor electrodes possess typical pseudocapacitance characteristics, with an acceptable specific capacitance of ~251 F/g at 1 A/g and long-term cycling stability (90% after cycling 5000 times at 3 A/g). Moreover, the asymmetric and flexible supercapacitor composed of Co3O4@C and activated carbon is further assembled, and it can drive the red LED for 6 min.Keywords:ZIF-67;Co3O4nanosheet;in situ growth;Co3O4@C;supercapacitor
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PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Li-hu Qian,Wei-wei Dong,Hai-bin Li,Xiaojie Song,Yi Ding
The development of economical, efficient and stable non-noble metal catalysts plays a key role in electrocatalytic hydrogen evolution . NiCo 2 S 4 has been proved to be an efficient non-noble catalyst, to further improve its electrocatalytic performance is a meaningful work. In this paper, the effects of Fe doping on electrochemical performance of NiCo 2 S 4 is investigated. The Fe-doped NiCo 2 S 4 catalyst is prepared by a facile solvothermal method with metal-organic-framework (MOF, ZIF-67) as template, and it exhibits an improved hydrogen evolution reaction (HER) performance with an overpotential of 181 mV at 10 mA cm −2 , a Tafel slope of 125 mV dec −1 compared with that of NiCo 2 S 4 (252 mV overpotential and 149 mV dec −1 Tafel slope). The combination of improved conductivity, mesopores architecture retained with the ZIF-67 template, which result the reduced internal resistance, enhanced charge transportation as well as large electrochemical double-layer capacitance. This work provides an effective and synergistic strategy for fabricating NiCo 2 S 4 -based catalysts toward electrochemical water splitting.
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INORGANIC CHEMISTRY COMMUNICATIONS
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2023
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IF 3.8
Ting Liu,Ling Wang,Yang Yu,Zhuo Zhang,Zelong Duan,Yawen Li,Chencan Li
Zeolitic imidazole framework-67 (ZIF-67) was demonstrated to exhibit intrinsic peroxidase-like activity by using 3,3′,5,5′-tetramethylbenzidine (TMB) as a chromogenic substrate. However, due to the inherent defects in the chemical stability and thermal stability of ZIFs, the peroxidase-like activity of ZIF-67 was severely affected. Therefore, establishing a simple and effective method to enhance the stability of ZIF-67 is necessary. ATP was found to improve the catalytic activity of ZIF-67. On the one hand, compared with ZIF-67, the catalytic efficiency of ZIF-67/ATP increased by 796 %, 5010 % and 570 % at 25 °C, 30 °C and 40 °C, respectively. In addition, the catalytic activity of ZIF-67/ATP was also greatly enhanced at pH-4. On the other hand, compared with ATP, the catalytic rate of ZIF-67/ATP increased by 364 % after 10 min of incubation. Inspired by the high catalytic activity of ZIF-67/ATP, we used the ZIF-67/ATP peroxidase-like system for colorimetric detection of glutathione with the limit of detection (LOD) of 0.46 μM. Furthermore, the proposed method provides a perspective on stabilizing the structures of ZIFs and developing a simple and efficient detection method.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Yu Liu,Linlin Qin,Yiming Qin,Tong Yang,Haoran Lu,Yulong Liu,Qiqi Zhang,Wenyan Liang
Nitrogen-containing heterocyclic compounds (NHCs) are hazardous, toxic, and persistent pollutants, thereby requiring urgent solutions. Herein, ZIF-67 was compounded with powder-activated carbon (PAC) to prepare Co/NC/PAC (NC i.e. nitrogen-doped carbon) particle electrodes for the electrocatalytic treatment of pyridine and diazines . Co/NC/PAC reflected the confinement of Co 3 O 4 /CoN/Co 0 into the N-doped graphitic-carbon layer to generate both pyrrolic-N and graphitic-N active sites. Under the optimal conditions (0.3 A, 12 mL min −1 , and initial pH 7.00), the degradation of four NHCs realized 90.2–93.7% efficiencies. The number and position of N atoms in NHCs directly affected the degradation efficiency. The following increasing order of facilitated degradation was recorded: pyridazine < pyrimidine < pyrazine < pyridine. The as-obtained Co/NC/PAC possessed the direct redox effect on NHCs, achieving fast electrocatalytic rate. Species like ·OH and H* were detected in Co/NC/PAC system with contributions to NHCs degradation estimated to 24% and 34%, respectively. Density functional theory (DFT) calculations revealed H* susceptible to attacking the N position, while the meta-position of C was subject to hydroxyl radical (·OH) addition. Overall, degradation of NHCs was achieved by hydro-reduction, oxidation , ring opening cleavage, hydroxylation, and mineralization. Ring-cleavage and mineralization of NHCs provided a novel electrochemical strategy to refractory wastewater treatment .
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PubMed
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JOURNAL OF MEMBRANE SCIENCE
·
2021
·
IF 8.742
Caijiao Yu,Yueyao Liang,Wenjuan Xue,Zhengqing Zhang,Xuemeng Jia,Hongliang Huang,Zhihua Qiao,Donghai Mei,Chongli Zhong
Metal-organic framework (MOF) membranes have significant potential for use in efficient gas separation. However, fabricating polymer substrate-supported ultra-thin MOF membranes with no defects remains a challenge. Herein, we proposed an in situ interface self-repair strategy for fabricating ultra-thin and defect-free ZIF-67 membranes for the first time. This was realized by preparing a polyvinyl alcohol (PVA)-Co 2+ interfacial layer containing a Co 2+ ion layer and a PVA-Co 2+ complex layer. The PVA-Co 2+ interfacial layer released Co 2+ ions and acted as a metal source to form ZIF-67 membranes by reducing the coordination rate of Co 2+ ions with 2-methylimidazole. The embedded Co 2+ ions functioned as anchor sites for the nucleation of ZIF-67 membrane assisted by the interface-enhanced deprotonation of 2-methylimidazole. Especially, the slow release of Co 2+ ions from the PVA-Co 2+ interfacial layer facilitated self-repair of defects to form a continuous and dense MOF layer. ZIF-67 membranes, 80-280 nm thick, were successfully synthesized and demonstrated unprecedented CO 2 permeance and good CO 2 /N 2 selectivity. This work provides a promising strategy for the fabrication of ultra-thin and defect-free MOF membranes on polymeric support layers for use in practical applications.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Qian Zhou,Bo Jin,Ping Zhao,Shijin Chu,Rufang Peng
Radioactive pollution is extremely harmful to humans and the environment and is difficult to manage. Therefore, finding an economical and efficient adsorbent for the treatment of uranium-contaminated wastewater is urgent. A composite carbon aerogel (CNQDs/rGO) was prepared by a simple one-step hydrothermal method by using CNQDs and graphene oxide as monomers. The ZIF-67 crystal was directly deposited on the template (expressed as CNQDs/rGO/ZIF-67 carbon aerogel (CGZCA)). The combination of CNQDs and graphene can not only graft some target groups (–OH, –COOH, and –NH-) onto the surface of 3D graphene carbon aerogels to promote adsorption, but also transform the zeta potential of rGO/ZIF-67 from positive to negative, which is more conducive to the adsorption process. The material observed by SEM and TEM shows that ZIF-67 and CNQDs are distributed on the carbon aerogel. The relationship of the adsorption of CGZCA to UO 2 2+ with contact time and initial concentration is examined. Results show that the adsorption of UO 2 2+ follows a pseudo-second-order kinetic model (R 2 = 0.999), and is consistent with the Langmuir adsorption isotherm model (R 2 = 0.991). The adsorption mechanism of the prepared adsorbent to UO 2 2+ is studied by XPS. Various parameters are studied in detail in the static adsorption experiment, and the removal of uranyl by adsorbents in different water bodies is simulated. In addition, dynamic adsorption behavior and adsorption effect of CGZCA on UO 2 2+ are investigated, which provides an appropriate reference basis for practical applications. Results show that the prepared ternary composite carbon aerogel is expected to be used in the extraction of uranium in wastewater and large-scale industrial production applications.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
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IF 3.573
Baozhong Lü,Weijie Qi,Mingsheng Luo,Qinglong Liu,Lin Guo
The preparation of highly active and stable catalysts for syngas conversion is a major challenge for Fischer–Tropsch synthesis (FTS). Herein, we report a strategy to prepare a highly dispersed Co-embedded porous carbon nanocage (CoPCN) structure derived from a core–shell metal–organic framework (MOF) ZIF-8@ZIF-67 precursor. High Co loading (over wt 30%) is achieved while maintaining an optimal dispersion and particle size of the active Co phase when a ZIF-8@ZIF-67 is pyrolyzed at 920 °C. Besides, the porous channels and hollow structures of the CoPCN strengthen the diffusion of reactants and the hydrocarbon product, enhancing the C5+ selectivity and CO conversion. The CoPCN shows high stability in FTS with a CO conversion of 18.3%, 80.2% selectivity for long-chain hydrocarbons (C5+), and 8.9% selectivity for short-chain hydrocarbons (C2–C4) after 100 h time on stream. Compared with other MOF-derived FTS catalysts, CoPCN-920 can achieve higher C5+ selectivity at a lower reaction temperature. The present work uncovers the relationship between the porous structure and catalytic performance, providing an efficient method to prepare promising materials for enhanced FTS stability, activity, and selectivity.
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