MATERIALS CHEMISTRY AND PHYSICS
·
2023
·
IF 4.6
Qirun Wang,Yanjie Duan,Zhixiong Huang,Xiaowei Xu,Jichao Shi,Lin Lin,Sheng Han,Runping Jia,Shufang Chang,Dandan Wu
Electrocatalysts with densely exposed sites and high intrinsic activity are desired for high-efficiency oxygen evolution reaction (OER). In this paper, we report the microwave assisted solvothermal growth of NiMoO 4 nanoflowers on electrodeposited Ni(OH) 2 nanosheets , forming a high specific surface area (132.5 m 2 g -1 ) nanoflower-like NiMoO 4 /Ni(OH) 2 configuration supported on a conductive nickel foam (NF) substrate. The as-prepared NiMoO 4 /Ni(OH) 2 /NF behaved efficiently as a self-supported 3D catalyst electrode for alkaline OER, compared with commercial RuO 2 (298 mV overpotential at 10 mA cm −2 and Tafel slope of 88.6 mV dec −1 ), needing a low overpotential of 292 mV to attain 10 mA cm −2 , with a small Tafel slope of 85.0 mV dec −1 and good stability for 100 h running at 10 mA cm −2 in 1.0 M KOH. Aside from enlarged surface area for more exposed edge sites for catalysis, the modulated synergy between Ni and Mo atoms probably contributes to enhanced intrinsic activity. A more electronegative Mo increases the electron density of Ni, thus accelerating the deprotonation of intermediates and driving the transition from Ni to NiOOH, leading to modulated thermodynamics and kinetics for OER catalysis.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Jiajia Wang,Lizhi Wang,Du Zhang,You Wang,Jiawei Li,Fa Zhou,Jianhan Huang,You-Nian Liu
Herein, the covalently connected core–shell metal–organic frameworks (MOFs)@covalent-organic frameworks (COFs) hybrid materials were successfully constructed by coating the stable COF-OH shell on the NH 2 -MIL-125 core. The introduction of the NH 2 -MIL-125 core endowed the hybrid materials with high Brunauer–Emmett–Teller (BET) surface area ( S BET ) and abundant unsaturated metal sites. And the coating of COF-OH shell endowed the hybrid materials outstanding physicochemical stability and visible-light response, and suitable band gaps. Moreover, the thickness of the COF-OH shell was carefully adjusted according to the feeding amount of NH 2 -MIL-125. Impressively, the electron transfer pathway in the formed heterostructure was clarified and it was proven that a type-II heterojunction was generated between the MOFs and the COFs. The formed stable C N covalent bonds in the interfacial layer was beneficial to the photogenerated electron transfer and the electron-hole pairs separation, which greatly enhanced the CO 2 photocatalytic reduction. The product NH 2 -MIL-125@COF-3 exhibited the highest CO yield of 22.93 μmol·g −1 ·h −1 , about 2 times higher than NH 2 -MIL-125 (11.82 μmol·g −1 ·h −1 ) and 3 times greater than COF-OH (7.26 μmol·g −1 ·h −1 ). This work can provide helpful ideas for the careful design of the novel MOFs@COFs hybrid materials as well as useful exploration for the CO 2 photocatalytic reduction.
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Polymers
·
2023
·Vol. 15
·期 1
·248
·
IF 5
Yao Lu,Xuna Jin,Xiang Li,Minpeng Liu,Baolei Liu,Xiaodan Zeng,Jie Chen,Zhigang Liu,Shihua Yu,Yucheng Xu
Superparamagnetic Fe3O4particles have been synthesized by solvothermal method, and a layer of dense silica sol polymer is coated on the surface prepared by sol-gel technique; then La(OH)3covered the surface of silica sol polymer in an irregular shape by controlled in situ growth technology. These magnetic materials are characterized by TEM, FT-IR, XRD, SEM, EDS and VSM; the results show that La(OH)3nanoparticles have successfully modified on Fe3O4surface. The prepared Fe3O4@La(OH)3inorganic polymer has been used as adsorbent to remove phosphate efficiently. The effects of solution pH, adsorbent dosage and co-existing ions on phosphate removal are investigated. Moreover, the adsorption kinetic equation and isothermal model are used to describe the adsorption performance of Fe3O4@La(OH)3. It was observed that Fe3O4@La(OH)3exhibits a fast equilibrium time of 20 min, high phosphate removal rate (>95.7%), high sorption capacity of 63.72 mgP/g, excellent selectivity for phosphate in the presence of competing ions, under the conditions of phosphate concentration 30 mgP/L, pH = 7, adsorbent dose 0.6 g/L and room temperature. The phosphate adsorption process by Fe3O4@La(OH)3is best described by the pseudo-second-order equation and Langmuir isotherm model. Furthermore, the real samples and reusability experiment indicate that Fe3O4@La(OH)3could be regenerated after desorption, and 92.78% phosphate removing remained after five cycles. Therefore, La(OH)3nanoparticles deposited on the surface of monodisperse Fe3O4microspheres have been synthesized for the first time by a controlled in-situ growth method. Experiments have proved that Fe3O4@La(OH)3particles with fast separability, large adsorption capacity and easy reusability can be used as a promising material in the treatment of phosphate wastewater or organic pollutants containing phosphoric acid functional group.Keywords:superparamagnetic;Fe3O4@La(OH)3inorganic polymer;phosphate adsorption
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2022
·Vol. 39
·期 2
·219-223
·
IF 2.726
Xiao Long,Wu Huirong,Zhang Yong,Sun Hao,Zhang Wenchao,Lyu Fenglei,Deng Zhao,Peng Yang
O xygen evolution reaction(OER) plays a key role in the electrochemical conversion and storage processes, but the sluggish kinetics of OER strongly impedes its large-scale applications. We herein reported the in situ growth of Fe-benzenedicarboxylate(Fe-BDC) on Co(OH) 2 nanoplates[Fe-BDC/Co(OH) 2 ] that showed remarkably enhanced OER activity than the pristine Co(OH) 2 . The incorporation of Fe species could enhance the intrinsic OER activity of Co and BDC could increase the electrochemically active surface area(ECSA), thus resulting in dramatically enhanced OER activity. In situ Raman spectroscopy characterization disclosed that Fe-CoOOH reconstructed from Fe-BDC/Co(OH) 2 was the real active site for OER. This work highlights the significance of rational tailoring of the nanostructure and electronic structure of Co(OH) 2 and provides more opportunities for its widespread applications.
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Nanomaterials
·
2022
·Vol. 12
·期 22
·3972
·
IF 5.719
Xue-Zhi Song,Yu-Hang Zhao,Fan Zhang,Jing-Chang Ni,Zhou Zhang,Zhenquan Tan,Xiao-Feng Wang,Yanqiang Li
The oxygen evolution reaction (OER) is kinetically sluggish due to the limitation of the four-electron transfer pathway, so it is imperative to explore advanced catalysts with a superior structure and catalytic output under facile synthetic conditions. In the present work, an easily accessible strategy was proposed to implement the plant-polyphenol-involved coordination assembly on Co(OH)2nanosheets. A TA-Fe (TA = tannic acid) coordination assembly growing on Co(OH)2resulted in the heterostructure of Co(OH)2@TA-Fe as an electrocatalyst for OER. It could significantly decrease the overpotential to 297 mV at a current density of 10 mA cm−2. The heterostructure Co(OH)2@TA-Fe also possessed favorable reaction kinetics with a low Tafel slope of 64.8 mV dec−1and facilitated a charge-transfer ability. The enhanced electrocatalytic performance was further unraveled to be related to the confined growth of the coordination assembly on Co(OH)2to expose more active sites, the modulated surface properties and their synergistic effect. This study demonstrated a simple and feasible strategy to utilize inexpensive biomass-derived substances as novel modifiers to enhance the performance of energy-conversion electrocatalysis.Keywords:Co(OH)2;tannic acid;electrocatalyst;OER;coordination assembly
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Zhihui Wei,Jie Li,Lixia Yang,Siyu Liu,Haicheng Li,Mingxia Lu,Tiantian Ying,Yan Luo,Kexin Li,Zhenglin Chen,Xiuping Zhang,Shenglian Luo
Degradation of halogenated organic compounds using the electro-reduction process is a promising approach for advanced water treatment. In this work, antiferromagnetic Co 3 O 4 nanoparticles were first loaded on a uniform anodic porous TiO 2 surface through a hydrothermal strategy, then subjected to an electrochemical reduction, which transform from nanoparticle-shape to interconnected nanoflakes. Compared with the pristine Co 3 O 4 nanoparticles, the morphologically transformed Co 3 O 4 cathode features a porous interface with amorphous Co(OH) 2 and CoOOH shell, which favors the generation of abundant •OH radicals along with lower overpotential for reducing H + to H*. On account of the plentiful radicals and self-supporting nature, the resulting Co 3 O 4 cathode retains high activity for efficiently degrading Thiamphenicol in water, even after 10 h run, demonstrating remarkable durability. Moreover, it is adaptable in a wide pH window of 3 to 10, and effectual when the initial Thiamphenicol concentration increases from 0.5 to 50 mg/L regardless of the water background (tap water, lake water, or river water). This study delivers a profound cognition about the dynamic behaviors of Co 3 O 4 -based electrocatalysts applied in eliminating halogenated antibiotics.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Fangke Yu,Yang Yang,Yanfang Zhang,Yuwei Pan,Ying Zhang
The present study describes the coating of modified graphite felt (GF) with graphene (GE) and polyaniline (PANI). GF was doped with nitrogen atoms by a series of modification and electrolytic deposition . Tests of different types of N content and cathodic catalytic oxidation performance confirmed that the graphite N introduction promoted the production of H 2 O 2 in the 2e - process. Pyridine N catalyzed the H 2 O 2 decomposition to produce •OH. The amount of H 2 O 2 produced by GF, GF-GE, and GF-GE@PANI system was 11 mg L -1 , 70 mg L -1 , and 180 mg L -1 , respectively. The doping of graphene increased H 2 O 2 yield, and the electrolytic deposition of PANI converted H 2 O 2 to •OH rapidly. It was proved that the N atom provided by graphene was graphite N, which was the active catalytic site for the production of H 2 O 2 . The perfluorooctanoic acid (PFOA) removal at 180 min was 24.1% and 49.8% in the GF and GF-GE systems, respectively. The GF-GE@PANI system achieved 100% PFOA removal within 160 min. It was demonstrated that the enrichment of PANI with pyridine N provided many active sites for improving the conversion of H 2 O 2 to •OH and in-situ degrading organic pollutants , offering an alternative for wastewater treatment .
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Journal of Physical Chemistry C
·
2022
·
IF 4.177
Yanjun Yu,Chen Chen,Yiheng Liu,Hongliang Yu,Shuaijie Li,Yanan Xue,Ning Cai,Jianzhi Wang,Faquan Yu
Developing efficient and cost-effective bifunctional catalytic electrodes is of great importance to water splitting. In this study, hybrid Ni/Ni(OH)2-coated NiCo2O4 nanorods were grown on Ni foam (NF) by a facile growth–conversion–epitaxy approach. The epitaxial decoration of Ni/Ni(OH)2 composite could increase the intrinsic activity of NiCo2O4/NF and enhance the charge-transfer rate. This self-standing hierarchical nanohybrid with unique surface chemistry and interface engineering exhibits an excellent electrocatalytic performance. The optimized Ni/Ni(OH)2-NiCo2O4/NF only requires overpotentials of 53 and 235 mV to reach a current density of 10 mA cm–2 for HER and OER, respectively. The electrolyzer achieved 10 mA cm–2 at a low cell voltage of 1.51 V for water splitting. This work offers a new perspective for rationally designing electrocatalytic materials by surface decoration.
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Small
·
2022
·Vol. 18
·期 23
·2200548
·
IF 15.153
Meng-Meng Pan,Yu Ouyang,Yong-Li Song,Lu-Qin Si,Ming Jiang,Xu Yu,Li Xu,Itamar Willner
The synthesis and characterization of Au 3+ -modified UiO-67 metal-organic framework nanoparticles, Au 3+ -NMOFs, are described. The Au 3+ -NMOFs reveal dual oxidase-like and peroxidase-like activities and act as an active catalyst for the catalyzed generation of O 2 •− under aerobic conditions or •OH in the presence of H 2 O 2 . The two reactive oxygen species (ROS) agents O 2 •− and •OH are cooperatively formed by Au 3+ -NMOFs under aerobic conditions, and in the presence of H 2 O 2. The Au 3+ -NMOFs are applied as an effective catalyst for the generation ROS agents for antibacterial and wound healing applications. Effective antibacterial cell death and inhibition of cell proliferation of Staphylococcus aureus ( S. aureus ) and Escherichia coli ( E . coli ) bacterial colonies are demonstrated in the presence of the Au 3+ -NMOFs. In addition, in vivo experiments demonstrate effective wound healing of mice wounds infected by S. aureus , treated by the Au 3+ -NMOFs.
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ChemElectroChem
·
2022
·Vol. 9
·期 2
·e202101523
·
IF 4.782
Junye Zhang,Hao Guo,Fan Yang,Mingyue Wang,Tingting Zhang,Hao Zhang,Wu Yang
Graphical Ni-MOF derived CMs@Ni(OH) 2 /NiSe with a core-shell structure was designed. The obtained core-shell nanostructure material possesses a high contact area, excellent synergistic effect and can provide more reactive active sites. The application of Ni-MOF in supercapacitors has received widespread attention, but its poor conductivity and bad stability hinder its application. Therefore, Ni-MOF derived CMs@Ni(OH) 2 /NiSe with a core-shell structure was designed. Here, carbon microspheres (CMs) were explored as the conductive substrate to enhance the stability and in situ prepared Ni-MOF was anchored on the surface of CMs. Then, alkali-treatment and selenylation were carried out on CMs@Ni−MOF to improve stability and conductivity. The obtained core-shell nanostructure material possesses a high contact area, excellent synergistic effect and can provide more reactive active sites. The prepared CMs@Ni(OH) 2 /NiSe shows a higher specific capacitance (2106 F g −1 ) and excellent cycling performance with a capacitance retention of 95 % after 30000 cycles. Furthermore, the assembled CMs@Ni(OH) 2 /NiSe//AC device delivers a high energy density of 70.84 Wh kg −1 at the power density of 756.8 W kg −1 and maintains 100 % of the initial capacitance after 40000 cycles.
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Fundamental Research
·
2023
·
IF 6.2
Qian Hu,Taoyu Yang,Shanli Wang,Licong Xu,Minghua Wu,Deyou Yu,Kaixing Fu,Jinming Luo
Peracetic acid (PAA) has recently been considered a promising oxidant candidate for heterogeneous Fenton-like reactions; however, the main generation and contribution of organic radicals (R-O•) with unsatisfactory oxidation potential compromises wastewater decontamination efficiency. In this study, we demonstrate the rational design and synthesis of ultrafine FeO x nanocluster-anchored carbonaceous nanosheets (UFe-CN) for altering the PAA activation pathway from R-O• to •OH dominant process via in situ framework collapse carbonization of MIL-53(Fe). The constructed UFe-CN/PAA system effectively accelerated refractory micropollutant ( e.g. , p-nitrophenol (4-NP)) decomposition by the enhanced •OH formation (up to 65.24 μmol L − 1 ) under a wide pH range (3.0–9.0), outperforming the benchmark iron-based catalyst counterparts by 4.2–10.8 times. This outstanding Fenton-like catalytic activity of UFe-CN is primarily attributed to the significant improvement in electron mitigation, ca. 49 times higher than that of its MIL-53(Fe) counterpart, for interface catalysis reactions triggered by iron species cycling. Furthermore, to facilitate adaptive engineering, the organic pollutant removal efficiency could be easily tuned by varying several key treatment factors, including the initial pH, PAA concentration, and UFe-CN dosage. More importantly, the excellent practicality of UFe-CN/PAA was demonstrated by systematically evaluating the impact of the water matrix, catalyst regeneration capability, and wastewater treatment efficiency. Overall, this study provides a significant understanding of •OH-dominated PAA activation and an effective catalyst development paradigm to facilitate the practical application of PAA-based Fenton-like oxidation.
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NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 46
·期 3
·1158-1167
·
IF 3.591
Huan Fu,Huan Zhang,Guichun Yang,Jun Liu,Junyuan Xu,Peihuan Wang,Ning Zhao,Lihua Zhu,Bing Hui Chen
Catalysts of 0.54% (Pt, Rh, Pd or Ru)/Co(OH)2 and 1.23% Rh/Co(OH)2 were successfully synthesized via simple hydrothermal and precipitation methods for the selective hydrogenation of nitroarenes. It was found that 0.54% Rh/Co(OH)2 outperformed other catalysts, for example, 2-chloronitrobenzene hydrogenation (with a turnover frequency (TOF) of 575 h−1) under 3.0 MPa H2 at 100 °C for 1 h (much higher than that of 1.23% Rh/Co(OH)2; TOF, 398 h−1). Through characterization of the nanostructure (XRD, TEM, HRTEM, AC-STEM (spherical aberration-corrected scanning transmission electron microscopy), AC-STEM-EDX elemental mapping and line-scanning, H2-TPD, etc.), it was confirmed that Rh was dispersed in the form of single atoms and ultrasmall nanoclusters on Co(OH)2 for 0.54% Rh/Co(OH)2. Moreover, 0.54% Rh/Co(OH)2 also exhibited high selectivity for –NO2 hydrogenation for other selected nitroarene substrates hydrogenation reactions. This was mainly attributed to the presence of Rh as single atoms or super tiny nanoclusters in 0.54% Rh/Co(OH)2, leading to a significant increase in the number of active sites, beneficial adsorption of the –NO2-group at defect-rich Co(OH)2, and an interfacial synergy effect of Rh–Co(OH)2, thus improving the catalytic performance.
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