NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 48
·期 1
·228-236
·
IF 3.3
Yan Wang,Haoran Li,Daqing Chen,Danhua Ge,Xiaojun Chen
Herein, a simple solvothermal method was used to prepare a CuSx/g-C3N4 (CSG) heterojunction as an efficient oxygen activator containing sulfur vacancies (SVs). The as-prepared catalyst can activate oxygen to effectively degrade tetracycline (TC). The degradation rate of TC (20 mg L−1) reached 98.9% in 90 min over CSG (0.02 g L−1) under an air atmosphere, which maintained good performance within a wide pH range of 6–10. It was almost unaffected by any light source and water quality, indicating a highly efficient oxygen activator and good stability. Moreover, the trapping experiments and EPR results revealed that the main reactive oxygen species (ROSs) were singlet oxygen (1O2) and hydroxyl radicals (˙OH). CSG (4 : 1) enabled the activation of oxygen-produced ROS for removing TC even in the dark, which was in accordance with the EPR results. In addition, the CSG catalyst exhibited a good removal performance in practical wastewater treatment. Our study demonstrated that the CSG catalyst had the potential to remove organic pollutants from wastewater.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Jiani Zhang,Risheng Bai,Zhaochi Feng,Jiyang Li
Aiming to promote the activity of TS-1 zeolite in catalytic oxidative desulfurization (ODS), a general amide-assisted strategy was proposed to synthesize hierarchical TS-1 zeolite with rich and homogeneously distributed Ti(OH 2 ) 2 (OH) 2 (OSi) 2 species. Strong interactions between acrylamide (AM) and Si/Ti as well as self-polymerization of AM in synthetic gels change the zeolite formation process, thus to effectively construct Ti(OH 2 ) 2 (OH) 2 (OSi) 2 , promote Ti evenly distribution and form micro-mesopore structure. The activity of Ti(OH 2 ) 2 (OH) 2 (OSi) 2 was evaluated by ODS of refractory sulfur-containing compounds. The advantages of Ti(OH 2 ) 2 (OH) 2 (OSi) 2 over TiO 4 in substrate adsorption and reactive intermediate formation for ODS were further proved by theoretical calculations. By adjusting AM amount to optimize the Ti(OH 2 ) 2 (OH) 2 (OSi) 2 content and distribution, the obtained catalyst achieves 134.8 h -1 of turnover frequency and 100 % DBT removal at ten minutes, and maintains > 92 % removal after seven cycles at 333 K. This facile active-site construction strategy is promising to be extended to other heteroatom-containing zeolite catalysts.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·Vol. 141
·期 2
·e54774
·
IF 3
Wenyu Zhang,Yu Zhang,Weijie Cai,Dazhi Wang,Shaoyin Zhang
2,2,6,6-Tetramethylpiperidinium-nitroxide (TEMPO) is a mild and efficient catalyst, which is important in the industrial production of selective oxidation of alcohols to the corresponding aldehyde or ketone compounds. However, it is a challenge to recover the expensive TEMPO catalyst in homogeneous catalytic systems. In this study, a novel polymer-supported catalyst was prepared using 4-hydroxy-2,2,6,6-tetramethylpiperidin-1-oxy (4-OH-TEMPO) and polyaromatic ether sulfone (PAES). The successful grafting of 4-OH-TEMPO in PAES-C was demonstrated by 1 H nuclear magnetic resonance ( 1 H NMR) and Fourier transform infrared (FT-IR), load capacity can be calculated by elemental analysis (EA). BET and scanning electron microscopy (SEM) to depict the structure-performance relationship. Herein, SEM images revealed the existence of porous structure. This structure can effectively adsorb NO molecules to form a PAES-TEMPO/NO x catalytic system to selectively oxidize benzyl alcohol. The experimental results indicated the high activity, the subsequent benzyl alcohol oxidation cycle can reach more than 93% conversion without showing a large loss of selectivity. More importantly, the as-prepared catalyst exhibited the attractive recyclability (recovery rate is 98%). After 10 consecutive runs, no significant loss of conversion and selectivity was observed (the conversion rate of benzyl alcohol was more than 93% and the selectivity was more than 95%). This study might provide some recommendation on the development of highly efficient catalysts for alcohol oxidation.
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Surfaces and Interfaces
·
2023
·
IF 6.2
Lei Zhou,Xiangyu Xi,Haidong Li,Han Song,Qiong Mei,Yuankun Yang,Shu Chen,Qunwei Dai,Faqin Dong
Vanadium contamination has gained increasing attention around the world and it is urgent to develop feasible approach to tackle this growing pollution (e.g., vanadate). Herein, density functional theory (DFT) calculations combined with batch experiments were used to systematically evaluate the capacity of Mg(OH) 2 to adsorb vanadate , by investigating the impacts of different exposed facet and surface OH defect on the structure configurations, adsorption energy and the efficiency of vanadate adsorption. DFT calculations suggested that although the capacity of vanadate adsorption on the facets of Mg(OH) 2 would be obviously influenced by the formation of various coordination complex (e.g., monodentate, bidentate and tridentate) on each facet, the capacity for these facets of Mg(OH) 2 towards vanadate adsorption followed the order: (100) > (001). Moreover, such a vanadate adsorption was further enhanced by the presence of surface OH defect, owing to altered densities of states (DOS) of the adsorption site. Batch experiments verified the defect-rich Mg(OH) 2 was favorable to adsorb vanadate, and both (001) and (100) facet play the great roles. This molecular-level understanding of the facet-dependent and defect-enhanced adsorption behavior of Mg(OH) 2 toward vanadate provides a useful insight into designing and applying effective adsorbents for the removal of heavy metal oxyanions.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Hang Wang,Qing Sun,Yuanyuan Lin,Jian Zhang,Jiawei Sheng
Development of highly efficient and recyclable catalysts based on peroxymonosate (PMS) activation for the degradation of dangerous antibiotic contaminants was still a challenging topic. In this study, a highly efficient and recyclable heterogeneous Co(OH) 2 /ZnFe 2 O 4 (Co-ZF) catalysts derived from metal-organic frameworks (MOFs) were prepared by a facile alkaline solution hydrothermal method , a high specific surface area (100.4 m 2 g −1 ) and soft magnetic properties (Ms=25.3 emu g −1 ) composite material was obtained, and used for degrading norfloxacin (NOF) via PMS activation. The effects of temperature, alkali concentration, pH, initial NOF concentration, PMS and catalyst dosage on NOF degradation were discussed in detail. The results illustrated that the degradation rate of norfloxacin by the 3Co-ZF160 catalyst synthesized under 3 M NaOH and 160 ℃ hydrothermal conditions was 97.2%, after four consecutive cycles of degradation, the degradation rate of NOF by 3Co-ZF160 remained over 91% within 60 min. In contrast, the degradation rate of the Co 3 O 4 /ZnFe 2 O 4 (CZF-600) catalyst calcined at 600 ℃ was only 74% available. Furthermore, The results of radical quenching suggested that OH•, SO 4 • − , SO 5 • − and 1 O 2 functioned in the presence of the Co(OH) 2 /ZnFe 2 O 4 -PMS system. Eventually, NOF degradation pathways were tentatively proposed on the basis presented via LC-MS. The above results highlight that the practical application of Co(OH) 2 /ZnFe 2 O 4 heterogeneous catalyst in aqueous solution was of great significance.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Wenbo Li,Difei Xiao,Xueqin Gong,Xianbin Xu,Fahao Ma,Zeyan Wang,Peng Wang,Yuanyuan Liu,Ying Dai,Zhaoke Zheng,Yuchen Fan,Baibiao Huang
Electrocatalytic polyethylene terephthalate (PET) waste upgrading is crucial for developing a circular plastics economy and solving the energy crisis, but achieving efficient PET upgrading at an industrial-scale current density remains a formidable challenge. In our work, Ni-MOF@MnCo-OH catalyst was prepared by designing hierarchical heterostructure and incorporating the concept of multi-metal sites, wherein the Ni-MOF can be derived from PET plastic. Benefiting from the advantages of material design, the catalyst demonstrates excellent adsorption capabilities for both OH ad and ethylene glycol (EG), while also enhancing the electron transfer capability of Ni-MOF. We achieve a high Faradaic efficiency (∼80 %) during PET plastic upgrading at industrial-scale current density (300 mA·cm −2 at 1.43 V vs. RHE) with Ni-MOF@MnCo-OH. Moreover, through theoretical calculations and in situ Fourier transform infrared (FTIR) spectroscopy, we have further elucidated the mechanism of ethylene glycol oxidation reaction (EGOR). Notably, glycolic acid has been identified as a vital intermediate during the electrical oxidation of EG. This work provides a viable and eco-friendly approach to enhance the value of PET waste through sustainable means.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 28
·9721-9730
·
IF 4
Xinyu Liu,Lan Wang,Shan Ji,Vladimir Linkov,Qianqian Fu,Zhichao Li,Hui Wang
Due to their low cost and excellent electrocatalytic performance, nickel-based hydroxides are widely used as hydrogen evolution catalysts for large-scale hydrogen production by water electrolysis. In this study, a heterostructured composite with improved electron transport and modulated electron surface density was prepared by combining Ni(OH)2 with two-dimensional layered Ti3C2Tx (Ti3C2Tx-MXene). Ni(OH)2 nanosheets were formed on nickel foam (NF) substrates using acid etching, followed by the longitudinal growth of negatively charged Ti3C2Tx-MXene on positively charged Ni(OH)2/NF via electrophoretic deposition. The resulting structure facilitates spontaneous electron transfer from Ti3C2Tx-MXene to Ni(OH)2/NF by means of the Mott–Schottky heterostructure effect and establishes a continuous electron transport path which effectively increases the concentration of active sites, improving hydrogen evolution during water electrolysis. The obtained electrode is characterized by an HER overpotential of 66 mV (vs. RHE) and a Tafel slope of +105 mV dec−1 at a current density of 10 mA cm−2, combined with good electrochemical stability.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2023
·
IF 4.5
Defeng Qi,Ying Wang,Xinru Xu,Xiao Jiang,Mushtaq Ahmad,Zhao Chao,Zhenyi Yu,Meiling Lian,Yong Wang,Zhen Zhang
Nanostructured transition metal sulfides (TMSs) have attracted great attention owing to their superior electric conductivity and easy redox reaction properties in oxygen evolution reaction (OER) catalysts. However, the strong metal-metalloid bonds (M−S) and metalloid-metalloid (S S) bonds in the crystal structure of TMSs are difficult to break, which might result in the insufficient formation of electrocatalytically active metal hydroxide species on the surface and prevent the realization of their full OER potential. Herein, we demonstrate an approach by sculpting Co(OH) 2 on Co 3 S 4 nanotubes (Co 3 S 4 /Co(OH) 2 ) as highly reactive and stable electrocatalysts for efficient OER. The electron transfer between cobalt and sulfur and the pre-sculpted Co(OH) 2 promote the formation of rich hydroxide active species on the surface of Co 3 S 4 /Co(OH) 2 . The optimized Co 3 S 4 /Co(OH) 2 –0.8 catalyst possesses excellent electrocatalytic activity for OER in an alkaline medium, with a relatively low OER overpotential of 269 mV (at 10 mA cm −2 ) and a Tafel slope of 95.2 mV dec -1 . This work provides a new sight of designing TMS electrocatalysts for practical application in efficient water splitting.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Haili Tong,Yi Jiang,Lixin Xia
The CQDs + Ni(OH) 2 /BiVO 4 photoanode was fabricated by introducing CQDs with fluorescence and optical properties . The CQDs + Ni(OH) 2 /BiVO 4 photoanode exhibited a low water oxidation onset potential (∼0.2 V vs. RHE) and a photocurrent density of 3.05 mA cm −2 at a voltage of 1.23 V vs. RHE, which is about 2.5 times than that of the unmodified BiVO 4 electrode, and the charge injection efficiency is 65%. Surface dynamics test showed that CQDs + Ni(OH) 2 /BiVO 4 photoanode had higher charge transfer rate and lower charge recombination rate than BiVO 4 electrode. As a cheap and stable catalyst for water oxidation, Ni(OH) 2 combined with CQDs can effectively improve the migration of photogenerated electrons and holes, thereby improving the photoelectrochemical (PEC) water oxidation activity of the photoanode.
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JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY
·
2018
·Vol. 89
·期 2
·492-499
·
IF 1.745
Wang Li,Li Jing,Wang Meiri,Liu Yuanyuan,Cui Hongtao
Abstract 2D nanostructured Co 2+ -doped β-Ni(OH) 2 as electrode material for application in redox-type supercapacitors was synthesized by a strategy of nickel complex template. The 2D Co 2+ -doped β-Ni(OH) 2 was produced by the in situ reaction of 2D Co 2+ -doped template in strong alkaline electrolyte solution during electrochemical measurement. Due to the large interface and the promoted conductivity induced by Co 2+ doping, the Co 2+ -doped β-Ni(OH) 2 exhibited high electrochemical performance. It had high specific capacitance of about 2100 F g –1 at low current density of ~2 A g −1 . It also exhibited excellent high rate performance (1259 F g –1 at high current density of 41.7 A g −1 ), much higher than the undoped sample. The results in this work indicated that the Co 2+ -doped β-Ni(OH) 2 could be used as an effective electrode material in redox supercapacitors.
2D nanostructured Co 2+ -doped β-Ni(OH) 2 as electrode material for application in redox-type supercapacitors was in situ synthesized by a strategy of nickel complex template. Due to the large interface and the promoted conductivity induced by Co 2+ doping, the as-synthesized material exhibited excellent high rate electrochemical performance.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2018
·Vol. 29
·期 9
·7692-7700
·
IF 2.324
Hu Zhen,Guo Haiyong,Zhao Li,Wu Yadan,Wang Shimin,Wan Li
A double-layer composite film (DLCF) that consists of upconversion composite La(OH) 3 :Er 3+ /Yb 3+ +P25 (UC + P25) as underlayer and large TiO 2 spheres (LS-TiO 2 ) as overlayer is designed as the photoelectrode of dye-sensitized solar cells (DSSCs). The upconversion luminescent material La(OH) 3 :Er 3+ /Yb 3+ can convert near-infrared region to visible light to improve the light absorption, and LS-TiO 2 has been used as light-scattering layer to increase the optical length in the film and enhance light harvesting. The DLCF with lower absorbed dye achieved the highest conversion efficiency due to the synergistic effect of the upconversion luminescent layer and the light-scattering layer, and with an optimum mixing ratio, a conversion efficiency of 9.24% is attained, which is a significant improvement of 68.3% compared with the pure P25 film photoelectrode.
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Frontiers in Chemistry
·
2018
·
IF 4.155
Li Yinong,Tian Chen,Liu Weizhen,Xu Si,Xu Yunyun,Cui Rongxin,Lin Zhang
Nano-Mg(OH)2 is attracting great attention as adsorbent for pre-concentration and recovery of rare earth elements (REEs) from low-concentration solution, due to its superior removal efficiency for REEs and environmental friendliness. However, the nanoparticles also cause some severe problems during application, including aggregation, blockage in fixed-bed column, as well as the difficulties in separation and reuse. Herein, in order to avoid the mentioned problems, a carbon cloth (CC) supported nano-Mg(OH)2 (nano-Mg(OH)2@CC) was synthesized by electrodeposition. The X-ray diffraction and scanning electron microscopy analysis demonstrated that the interlaced nano-sheet of Mg(OH)2 grew firmly and uniformly on the surface of carbon cloth fibers. Batch adsorption experiments of Eu(III) indicated that the nano-Mg(OH)2@CC composite maintained the excellent adsorption performance of nano-Mg(OH)2 toward Eu(III). After adsorption, the Eu containing composite was calcined under nitrogen atmosphere. The content of Eu2O3 in the calcined material was as high as 99.66%. Fixed-bed column experiments indicated that no blockage for Mg(OH)2@CC composite was observed during the treatment, while the complete blockage of occurred to nano-Mg(OH)2 at an effluent volume of 240 mL. Moreover, the removal efficiency of Mg(OH)2@CC was still higher than 90% until 4,200 mL of effluent volume. This work provides a promising method for feasible application of nanoadsorbents in fixed-bed process to recycle low-concentration REEs from wastewater.
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