APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Sijia Liu,Xifei Zhou,Changqing Yang,Chaohai Wei,Yun Hu
The extensive use of sacrificial agents and the low carrier separation and utilization efficiency remain important factors limiting the development of photocatalytic hydrogen production . We report a three-layered, dual-functional photocatalysts of Cu atomics@UiO-66-NH 2 (U6N)/ZnIn 2 S 4 nanosheets (ZIS), for the simultaneous production of photocatalytic hydrogen and degradation of organic pollutants . When common and highly toxic organic pollutants (phenolic compounds and antibiotics) were substituted for the sacrificial agents, Cu@U6N/ZIS exhibited superior sustained hydrogen production, approximately 28 times greater than that of pure ZIS. The experimental results suggested that the window size of U6N (< organic pollutants molecular size) separates the reaction sites of organic pollutants oxidation and reduction of hydrogen ions (H + ), thereby achieving spatial separation of redox sites. Besides, the structure of Cu@U6N/ZIS, which was anchored Cu within U6N and encapsulated by ZIS nanosheets, forming Z-type heterojunctions, achieved the control of the directional transfer of photogenerated electrons. And the coupled system can effectively enhance water quality by reducing the biological toxicity of the wastewater. This study suggests new avenues for environmental restoration and non-fossil fuel production.
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高影响因子
FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Yu Tang,Yi Cui,Gaosheng Ren,Ke Ma,Xiaoxun Ma,Chengyi Dai,Chunshan Song
In this study, the copper-mordenite zeolite (Cu-MOR) and non-thermal plasma were used to produce methanol and hydrogen from methane and water at low temperature (120 °C) without CO 2 formation. Energy efficiency for methanol and hydrogen were 68.8 mmol·kJ −1 and 562.3 mmol·kJ −1 , respectively, and the selectivity of methanol in liquid products reached 86%. The reaction mechanism likely involves methane being excited to methyl (·CH 3 ) and hydrogen radicals (·H) under DBD plasma conditions, which can then adsorb on the catalyst surface at the Cu 2 -(μ-O) 2+ active sites, accompanied by water co-adsorption to facilitate formation and desorption of methanol. XPS analysis showed that with the prolongation of reaction time, Cu 2 -(μ-O) 2+ was reduced to Cu + and Cu(II) hydroxide, and the catalyst had carbon deposition , resulting in the decrease of catalytic activity . It is also worth noting that in an oxygen atmosphere, Cu 2 -(μ-O) 2+ regenerates rapidly and eliminates catalyst carbon deposits . Trace oxygen was introduced into the reactor, and the reaction was carried out for 30 h, and the catalytic activity did not decrease.
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Journal of Cleaner Production
·
2023
·
IF 11.1
Shan Peng,Xiaoxin Chen,Xin Rong,Haobo Ma,Chenyang Zhao,Kyongjin Pang
Microplastics (MPs) are ubiquitous in aquatic and terrestrial environment, which pose serious threat to ecosystem and human health. Although many approaches have been developed, most of them showed low efficiency and long processing cycle. Herein, a cost-effective and eco-friendly coated sponge (HDTMS/CuCo-LDHs/PDA@Sponge) was successfully fabricated for the first time via the supersaturated coprecipitation methods, integrating of multistage lamellar layered hydroxides (LDHs) structure, polydopamine (PDA) adhesive layer , and hydrophobic agent. Among them, (i) the complexation of PDA can enhance the growth of CuCo-LDHs, (ii) the large surface area of CuCo-LDHs provided plentiful action sites for linkage of PDA and HDTMS molecules, thus self-strengthened the coating much more firmly, (iii) the cooperation of three buildings significantly promoted the adsorption capacity of coatings to various pollutants. The finally coated sponge showed mechanically durable, superhydrophobicity, salt tolerance, and antibacterial activity, which could efficiently and synchronously absorb MPs (polypropylene and polyethylene), dyestuff, and tiny oil, and the removal rates remained almost 100% for these pollutants. Moreover, the large-scale coated sponge (9 cm × 6 cm × 1 cm) could simultaneously adsorb almost 100% MPs (40 mg/L), Sudan Ⅲ (10 mg/L), and dodecane (20 mL/L) within 1 min. The absorption energy between the coatings and MPs were −1699 kcal/mol for PP and −932.8 kcal/mol for PE, respectively. The adsorption mechanism was ascribed to multiple forces, including electrostatic interaction, capillary attraction, hydrogen bond , p-π conjugation, Van der Waals force , lipophilicity, complexation, surface adhesion of PDA, and lipophilicity of HDTMS clusters. The developed superhydrophobic sponge will be a novel strategy to purify wastewater, especially for the high-salinity and microbial-rich marine environment.
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APPLIED SURFACE SCIENCE
·
2023
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IF 6.7
Jie Mei,Guangya Hou,Huibin Zhang,Qiang Chen,Huazhen Cao,Yiping Tang,Jianli Zhang,Guoqu Zheng
In multifunctional catalysts, Ni-based alloys and compounds can be used for methanol oxidation reaction (MOR) and urea oxidation reaction (UOR). Herein, the porous dendritic NiCu@PPy/316L stainless steel mesh (SSM) electrode is prepared by dynamic hydrogen bubble template electrodeposition, followed by cyclic voltammetry electrodeposition of polypyrrole (PPy) conductive polymer on the electrode surface. Among them, dynamic hydrogen bubbles successfully assisted the formation of porous structures in the Ni-based deposition layer. In addition, the morphology of the resulting Ni-based layer further evolves from particle stacking to dendritic with high specific surface area with Cu doping. Eventually, 2-NiCu/SSM achieves current densities of 294.5 mA·cm −2 (MOR) and 278.6 mA·cm −2 (UOR) at 0.8 V, respectively. The PPy coating prevents the agglomeration of NiCu particles in the catalytic layer and further improves the persistence of the electrochemical performance. After 2000 cycles, the current densities of 2-NiCu @PPy/SSM in the new electrolyte are maintained at 89.1% (MOR) and 94.8% (UOR) of the original value, with a 10% increase for MOR and a 7% increase for UOR compared to the sample without PPy coating (2-NiCu /SSM).
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POLYMER DEGRADATION AND STABILITY
·
2023
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IF 5.9
Yaxuan Wang,Jinyong Ren,Mingyu Ou,Jiahui Cui,Haocun Guan,Richeng Lian,Chuanmei Jiao,Xilei Chen
To meet the demands of reducing the serious illness caused by the growth of bacteria and the severe life-threatening due to interior fabric fire, the attention to antibacterial flame-retardant cotton fabrics has reached an unprecedented height. In this work, a simple step-by-step dip-coating method was applied for the multifunctional cotton based on epichlorohydrin-modified aramid nanofibers (AEP), ionic liquid (IL), and CuSO 4 . Cot/AEP/IL/Cu exhibited low flammability with a limiting oxygen index (LOI) improving from 18.5% to 28.5% and high flame retardancy (e.g., ∼43.7% and 41.7% decline in peak heat release rate (pHRR) and total heat release rate (THR)). Noticeably, the Cot/AEP/IL/Cu revealed conspicuous smoke suppression and toxic reduction property compared with Cot/AEP/IL (e.g., ∼77.0% decline in peak smoke release rate (pSPR) and 40.5% in total CO production (TCOP)). In addition, the antibacterial property of treated cotton was investigated by the agar diffusion plate method. Due to the presence of Cu ion, Cot/AEP/IL/Cu remarkably restrains the activity of E. coli and S. aureus. This work prepared a multifunctional cotton fabric integrated with flame-retardant, smoke suppression, toxicity reduction, and antibacterial in a straightforward way, which endows promising applications in many fields.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Ruilu Yang,Qi Zhang,Jian Shi,Yaping Zheng,Dechao Wang,Jian Zhang,Siyuan Liu,Zhuting Fu
The first example of a magnetic loading functional porous liquid (PL) by employing hollow silicon dioxide (HS) loaded with Fe 3 O 4 as the porous guest, (3-glycidyloxypropyl) trimethoxysilane (KH560) and polyetheramine M2070 as hindered sterically solvents was demonstrated in this paper. This nanoadsorbent (Fe 3 O 4 @HS-PL) was prepared for the decontamination of aqueous solutions from Cu(II) and Pb(II) heavy metals. The hindered sterically solvents ( i.e. , the flexible oligomer chains) endow the Fe 3 O 4 @HS porous guest with a superior flowing behavior at ambient temperature. Various approaches were applied to confirm the morphology, structure and properties of the resultant Fe 3 O 4 @HS-PL. More significantly, the adsorption behavior of Cu(II) and Pb(II) in aqueous solution by Fe 3 O 4 @HS-PL was studied in detail. As expected, combined with the cavity structure from porous guest and amine groups from flexible organic flow layer, Fe 3 O 4 @HS-PL exhibited excellent adsorption capacities of 322.58 and 357.14 mg·g −1 for Cu(II) and Pb(II), respectively, at 298 K, pH 8 and initial concentration of 20 mg·L -1 . The obtained HS and Fe 3 O 4 in Fe 3 O 4 @HS-PL magnetic nanoadsorbent presented average particles size ascertained to be ca. 200 nm and 30 nm, respectively. Moreover, the Freundlich model and pseudo-first-order model has described the adsorption process and adsorption kinetics . The parameters in thermodynamic experiment signified the spontaneity and endothermic properties of the adsorption. Moreover, magnetic loading endowed the Fe 3 O 4 @HS-PL with a superior regeneration performance. A variety of mechanisms containing coordination interaction, porous guest absorption, electrostatic interaction , steric effect and entropy are simultaneously realized in this novel adsorption system. Therefore, the introduction of PLs adsorbents into heavy metal adsorption systems through the construction of PLs materials by magnetic loading and surface amination is of great significance in the field of heavy metal adsorption, eventually starting a new time of pushing forward the development of novel adsorbents for decontamination of aqueous solutions from heavy metal ions.
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Molecular Catalysis
·
2023
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IF 4.6
Bo Li,Haijun Guo,Zhen Xiong,Lian Xiong,Shimiao Yao,Mengkun Wang,Hairong Zhang,Xinde Chen
γ-valerolactone (GVL) is a sustainable chemical, which can be obtained by hydrogenation of levulinic acid (LA) and levulinate. Herein, we reported a solvent-free hydrogenation of butyl levulinate (BL) to GVL and 1,4-pentanediol (1,4-PDO) over a skeletal Cu-Al-Zn catalyst. The skeletal Cu-Al-Zn catalyst was prepared from Devarda's alloy by alkali leaching and the catalyst was characterized by different analysis methods. The aluminum in the Devarda's alloy was dissolved by sodium hydroxide in the leaching process and many active Cu atoms were generated on the catalyst surface and the skeletal Cu-Al-Zn exhibited many micrometer-scale irregular particles with rough surface. The skeletal Cu-Al-Zn catalyst showed the excellent performance in the solvent-free hydrogenation of BL to GVL under constant hydrogen pressure (5 wt% catalyst loading, 180°C, 6 MPa of H 2 , 6 h): the LA conversion was 100%, the GVL yield was 74.75% and the 1,4-PDO yield was 25.63%. Moreover, the catalyst showed stable performance and it was reusable up to 5 times without apparent loss of activity. A stable hydrogen pressure with Zn would suppressed the dehydration of 1,4-PDO.
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MATERIALS CHEMISTRY AND PHYSICS
·
2023
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IF 4.6
Li Zheng,Song Luo,Sijie Yang
Carbon steel is a widely used metallic material. It is prone to corrosion. In this study, we designed and fabricated a superhydrophobic layer with corrosion resistance for protection of carbon steel substrate. Multiple layers were formed that acted as barriers to protect the substrate from corrosion. This superhydrophobic layer reduced the contact area between the substrate and the corrosive medium owing to the superhydrophobicity. The experimental results showed that a copper layer uniformly covered the carbon steel substrate, and the outer surface of the copper layer was converted into copper oxide , which had a multi-scale structure. The Cu/CuO double layer was modified with stearic acid (SA) to form a Cu/CuO@SA superhydrophobic layer. The superhydrophobic layer exhibited a high water contact angle (up to 160°) and a low sliding angle (<3°). The superhydrophobic layer also exhibited repulsive effect to salt, acidic and alkaline solutions. Atmospheric stability test and UV irradiation test were conducted and the results indicated that the superhydrophobic layer was stable throughout the test period. The corrosion potential of the superhydrophobic sample was −0.18 V and the corrosion current density was 7.72 × 10 −7 A cm −2 , which was one order of magnitude lower than that of the carbon steel substrate. These results indicate that the superhydrophobic sample had a low corrosion tendency and corrosion rate. The polarization resistance and impedance modulus of the superhydrophobic sample were two orders of magnitude higher than the bare steel sample, indicating corrosion resistance and effective protection to the carbon steel substrate.
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Journal of Energy Chemistry
·
2023
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IF 13.1
Mengxia Li,Tianxi Zheng,Dongfei Lu,Shiwei Dai,Xin Chen,Xinchen Pan,Dibo Dong,Rengui Weng,Gang Xu,Fanan Wang
The electrochemical hydrogenation of HMF to BHMF is an elegant alternative to the conventional thermocatalytic route for the production of high-value-added chemicals from biomass resources. In virtue of the wide potential window with promising Faradic efficiency (FE) towards BHMF, Cu-based electrode has been in the center of investigation. However, its structure–activity relationship remains ambiguous and its intrinsic catalytic activity is still unsatisfactory. In this work, we develop a two-step oxidation–reduction strategy to reconstruct the surface atom arrangement of the Cu foam (CF). By combination of multiple quasi-situ/in-situ techniques and density functional theory (DFT) calculation, the critical factor that governs the reaction is demonstrated to be facet effect of the metallic Cu crystal: Cu(110) facet accounts for the most favorable surface with enhanced chemisorption with reactants and selective production of BHMF, while Cu(100) facet might trigger the accumulation of the by-product 5,5′-bis(hydroxymethy)hydrofurion (BHH). With the optimized composition of the facets on the reconstructed Cu(OH) 2 -ER/CF, the performance could be noticeably enhanced with a BHMF FE of 92.3% and HMF conversion of 98.5% at a potential of −0.15 V versus reversible hydrogen electrode (vs. RHE) in 0.1 M KOH solution. This work sheds light on the incomplete mechanistic puzzle for Cu-catalyzed electrochemical hydrogenation of HMF to BHMF, and provides a theoretical foundation for further precise design of highly efficient catalytic electrodes.
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MOLECULES
·
2023
·Vol. 28
·期 12
·4630
·
IF 4.6
Qing Li,Yumeng Guo,Xiangyi He,Guangli Li
The sensitive and accurate determination of glyphosate (Glyp) is urgently demanded because it is closely correlated with human health and environmental safety. In this work, we proposed a sensitive and convenient colorimetric assay by employing copper ion peroxidases for the detection of Glyp in the environment. Free Cu(II) ions displayed high peroxidase activity and can catalytically oxidize the colorless 3,3′,5,5′-tetramethylbenzidine (TMB) into blue oxTMB, resulting in an obviously visible discoloration reaction. Once the Glyp is added, the ability of copper ions to mimic peroxidase can be largely suppressed because of the generation of Glyp–Cu2+chelate. The favorable selectivity and sensitivity were demonstrated in the colorimetric analysis of Glyp. Furthermore, this rapid and sensitive method was successfully applied in the accurate and reliable determination of glyphosate in the real sample, holding promising applications in pesticide determination in the environment.Keywords:label-free;colorimetric analysis;copper ions;peroxidase-mimicking activity;glyphosate
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PubMed
高影响因子
Materials Today Chemistry
·
2022
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IF 7.613
Mingzhen Huang,Siyuan Hu,Dongren Cai,Guowu Zhan
It is a significant method to prepare highly dispersed polymetallic oxides using in-situ doping metal organic frameworks as precursors. Herein, a series of straw-like W/Cu/Ce trimetallic oxides were prepared by using phosphotungstic ionic liquid@Ce-based metal organic framework adsorbing with copper acetylacetonate as precursors. The effect of W content on catalytic activity of W/Cu/Ce trimetallic oxides for carbon monoxide (CO) oxidation was well-investigated. Comprehensive characterization methods and density functional theory calculations were adopted to reveal the property changes of Cu/CeO 2 catalyst by the addition of W. The results demonstrated that W, Cu, and Ce are highly dispersed in the prepared W/Cu/Ce trimetallic oxides, and adding proper amount of W can improve the activity of the catalyst. H 2 temperature-program reduction profiles, X-ray photoelectron spectroscopy, in-situ diffuse reflectance infrared Fourier transform spectroscopy , and density functional theory calculations clearly revealed that after the addition of W, the strength of Ce-O bond is weakened, the oxygen vacancy is increased, and the adsorption of CO is enhanced, respectively, which are vital reasons for its high catalytic activity. In addition, the CO oxidation reaction pathway over prepared W/Cu/Ce trimetallic oxides based on the Mars-van Krevelen mechanism was studied, and the results exhibited that CO can wrest the lattice oxygen of W/Cu/Ce trimetallic oxides to form CO 2 , which is also proved to be the rate-determining step in reaction process.
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Small
·
2023
·Vol. 19
·期 18
·2207240
·
IF 13.3
Yuanmeng Zhao,Yunhao Jiang,Yan Mo,Yueming Zhai,Juejing Liu,Andrew C. Strzelecki,Xiaofeng Guo,Changsheng Shan
It is critical to develop high-performance electrocatalyst for electrochemical nonenzymatic glucose sensing. In this work, a single-atom Pt supported on Cu@CuO core–shell nanowires (Pt 1 /Cu@CuO NWs) for electrochemical nonenzymatic glucose sensor is designed. Pt 1 /Cu@CuO NWs exhibit excellent electrocatalytic oxidation toward glucose with 70 mV lower onset potential (0.131 V) and 2.4 times higher response current than Cu NWs. Sensors fabricated using Pt 1 /Cu@CuO NWs also show high sensitivity (852.163 µA mM −1 cm −2 ), low detection limit (3.6 µM), wide linear range (0.01–5.18 µM), excellent selectivity, and great long-term stability. The outstanding sensing performance of Pt 1 /Cu@CuO NWs, investigated by experiments and density functional theory (DFT) calculations, is attributed to the synergistic effect between Pt single atoms and Cu@CuO core–shell nanowires that generates strong binding energy of glucose on the nanowires. The work provides a new pathway for exploring highly active SACs for electrochemical nonenzymatic glucose sensor.
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高影响因子
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