DIAMOND AND RELATED MATERIALS
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2023
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IF 4.1
Yingjie Huang,Zuoyi Xiao,Shangru Zhai,Qingda An
The development of a simple and convenient method for synthesizing photocatalysts for the degradation of tetracycline remains a great challenge. In this work, a Cu-MoO 2 @C composite was successfully synthesized by a high-temperature carbonization of ammonium molybdate infiltrated copper alginate aerogel , which was obtained by curing a mixture of sodium alginate and ammonium molybdate using Cu 2+ ions. The photocatalytic properties of the prepared composites were evaluated by the degradation of tetracycline. The results showed that the introduction of Cu nanoparticles on the MoO 2 @C hybrid could significantly improve the catalytic performance, and the degradation rate of tetracycline reached 92.48 % after 60 min light exposure. Tetracycline's estimated photodegradation rate constant, which was 0.04013 min −1 , was 5 times more than that of the composite without Cu loading. Furthermore, the reaction mechanism was explored by electron spin resonance (ESR) test and free radical capture reagent. Intermediate products of tetracycline degradation were analyzed by liquid mass spectrometry (LC-MS).
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ELECTROCHIMICA ACTA
·
2023
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IF 6.6
Chunyan Fan,Zehao Zang,Xiang Li,Junfang Zhang,Ping Yang,Lanlan Li,Xiaofei Yu,Xiaojing Yang,Zunming Lu,Xinghua Zhang
Transition metal hydroxides have superior oxygen evolution reaction (OER) activity but poor hydrogen evolution reaction (HER) performance, which greatly limits the water splitting for hydrogen production. Herein, copper modification of sulfur doped Co(OH) 2 hybrid catalyst (Cu@S-Co(OH) 2 ) was prepared by one-step of electrodeposition method which can serve as efficient hydrogen evolution reaction catalyst. In the presence of sulfur and copper, Cu@S-Co(OH) 2 hybrid catalyst exhibits the best catalytic activity, showing ultralow overpotential of 42 mV at a current density of 10 mA cm −2 . Compared with Co(OH) 2 , the overpotential is improved by nearly 100 mV as well as enhanced stability. In addition, the active site poison experiments proved that the active center is cobalt metal. Combined with the adsorption strength of the catalyst for OH and H species, it is considered that both S and Cu can enhance the adsorption of OH for Co(OH) 2 , while S is contributed to the adsorption of H, and Cu can promote the desorption of H. This work provides a facile method and new insight to enhance the HER activity for transitional metal hydroxides via metal and non-metallic elements co-modulation.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Wen He,Jizhou Cao,Feiyu Guo,Zhihao Guo,Peiguo Zhou,Rui Wang,Shuang Liang,Qunyan Pang,Bairen Wei,Yue Jiao,Tripti Singh,Qiliang Fu
Heavy-metal pollution is a significant environmental issue that has raised global concern due to its harmful impact on humans and the natural ecosystem. Heavy metal pollution poses several challenges in terms of remediation, including low adsorption capacity and efficiency, scale-up issues and non-degradability. Here, we developed an eco-friendly tunable dual-wavelength absorption mesoporous wood aerogel (TDWA) for removal of Cu 2+ ions from wastewater based on wood nanotechnology and carboxylated functionalization treatment. Nanostructured pores generated from the cell walls with carboxyl groups due to the removal of most lignin/hemicellulose and 2,2,6,6-tetramethylpiperidine oxidation. Mechanical compression was parallelly applied to the transverse direction of TDWA resulted in removing micron-scale cell cavity and intercellular, which significantly improved the dynamic adsorption performance with an excellent Cu 2+ adsorption capacity of 115 mg g −1 . This value is superior to most wood-based adsorption membrane as wastewater mainly flowed through the continuous microfibril network in the cell wall. The double-layer mesoporous TDWA membrane (5 mm) possessed a favorable removal efficiency (99.83 %) even after 5-cyclic adsorption (92.34 %). The invented nanostructured TDWA membrane in the current study has promising potential to substitute the present plastic-based membrane in the realistic Cu 2+ adsorption because of the facile technology, renewability and high removal efficient, as well as the complete biodegradability.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Yi Li,Yanghan Chen,Tao Chen,Guoqiang Shi,Lin Zhu,Ye Sun,Miao Yu
Ethanol (C2H5OH) is an economically ideal C2 product in electrochemical CO2 reduction. However, the CO2-to-C2H5OH conversion yield has been rather low and the underlying catalytic mechanism remains vague or unexplored in most cases. Herein, by decorating small Cu2S nanocrystals uniform ly on Cu nanosheets, three desirable features are integrated into the electrocatalyst, including a relatively high positive local charge on Cu (Cuδ+), abundant interfaces between Cuδ+ and zero-valence Cu0, and a non-flat, stepped catalyst surface, leading to the promoted affinity of *CO, decreased *COCO formation barrier, and thermodynamically preferred *CH2CHO-to-*CH3CHO conversion. As a result, a high partial current density of ∼20.7 mA cm–2 and a Faraday efficiency of 46% for C2H5OH are delivered at −1.2 V vs reversible hydrogen electrode in an H-cell containing a 0.1 M KHCO3 solution. This work proposes an efficient strategy for the high-yield CO2-to-C2H5OH conversion, emphasizing the promise for the industrial production of alcohol and related products from CO2.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Chongchao Zhang,Hang Yin,Xiao Bai,Ziyin Yang
In this paper, we report a new strategy to activate the electrocatalytic activity of Cu to realize the non-enzymatic detection of hydrogen peroxide . The Ru-doped copper nanoparticles were prepared on the surface of carbon materials by direct pyrolysis of Ru in exchange for Cu-BTC metal-organic framework. The materials were characterized by transmission electron microscopy (TEM), energy dispersive spectroscopy (EDS) and x-ray diffraction (XRD). Surprisingly, Ru doping induced obvious lattice distortion of Cu nanoparticles , which made Cu nanoparticles exhibit excellent electrocatalytic activity for hydrogen peroxide reduction. The sensor based on Ru-doped Cu nanoparticles can detect hydrogen peroxide in a wide linear range from 0.01 mM to 5.55 mM. Moreover, as a hydrogen peroxide sensor, it has a high sensitivity of 327.14 µA·mM −1 ·cm −2 and a low detection limit of 8.9 µM. Therefore, Cu nanoparticles with the lattice distortion was demonstrated to be a potential material for hydrogen peroxide electrochemical sensor .
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Jingjing Niu,Zhe Xue,Jiuchao Tang,Saravanan Rajendran,Xinyu Zhang,Jiaqian Qin
Developing efficient, economic, and environment-friendly electrocatalysts to meet the industrialized hydrogen evolution reaction (HER) needs is highly desired for dealing with the energy crisis. Under the known premise, how to reasonably control the doping amount of copper greatly influences the structure and is one of the key factors affecting the performance of the catalyst. Herein, a series of Ni–Cu–C electrocatalysts are successfully synthesized through a simple electrodeposition method. The unique dendritic morphology can be obtained by adjusting the different glucose concentrations . DFT simulation reveals that the proper proportion of copper can significantly modulate the H adsorption-free energy Δ G H ∗ It can boost the intrinsic activity of Ni–Cu–C catalysts. NCC-3 delivers an overpotential of 87 mV and 165 mV in alkaline media at the current density of 10 mA cm −2 and 100 mA cm −2 , respectively and presents outstanding long-term stability for 50 h. Such excellent HER activity stems from a large ECSA area and better electron-transfer ability. The study presents a feasible way to control metal alloy catalysts' composition in the electrodeposition process .
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ACS Sustainable Chemistry & Engineering
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2023
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IF 8.4
Hong Du,Xiuyun Ma,Miao Jiang,Siyuan Zhao,Qi Fang,Xiumei Liu,Zongchao Conrad Zhang
Xylitol is a value-added health product from the hemicellulose component in biomass. In this work, highly efficient Cu–Ni/SiO2 catalysts are developed for the production of xylitol by means of xylose hydrogenation. The bimetallic catalysts exhibit higher activity compared to the corresponding monometallic nickel or copper catalyst and the currently used industrial Raney nickel catalyst. The bimetallic catalyst with a higher ratio of nickel to copper shows a better performance. The 5Cu15Ni/SiO2 catalyst exhibits a xylose conversion of 96% accompanied by higher than 99% selectivity to xylitol under the moderate conditions of 100 °C and 3MPa H2. The bimetallic catalysts show improved performances when they are activated at a low temperature. The apparent activation energies of xylose hydrogenation over the 5Cu15Ni/SiO2 and 20Ni/SiO2 catalysts are 16.6 and 25.2 kJ/mol, respectively. The formation of the Cu–Ni alloy leads to a lower activation energy and thus superior performance for xylose hydrogenation to xylitol.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Xiaoping Liu,Yunbo Zhai,Zhixiang Xu,Liming Liu,Wanying Ren,Yu Xie,Caiting Li,Yun Zhu,Min Xu
The high water content of sewage sludge increases the processing costs and hampers its further disposal. Fenton technology has proven to be efficient and been widely used to enhance sludge dewaterability, but it usually needs acidification and subsequent neutralization, thus consuming a lot of chemicals. It’s well documented that hydroxyl radicals produced in various Fenton or Fenton-like reactions play a crucial role in sludge dewatering. Based on the latest study, Cu + and Cu + /H 2 O 2 pretreatments for the enhanced dewaterability of sludge without extra pH adjustment were proposed. Results showed that Cu + with and without H 2 O 2 can significantly improve the dewatering performance of sludge, which was ascertained by a capillary suction time (CST) reduction rate of about 80 %. The proteins and polysaccharides in tightly-bound extracellular polymeric substance (TB-EPS) were decreased, while increased in soluble extracellular polymeric substance (S-EPS). In addition, a hydrophobic and porous surface was formed, and zeta potential increased after conditioned. These changes may release bound water and thus improve sludge dewaterability. The results of electron spin resonance and scavenging tests signaled that the Cu 3+ was mainly accountable for the dissolution of EPS, rather than the hydroxyl radicals ( OH). Our results substantiate and untangle a distinct reinforcement mechanisms for sludge dewatering by high valent copper (Cu 3+ ). This study demonstrates for the first time that Cu 3+ plays an important role in sludge dewatering, which has long been credited to hydroxyl radicals. It also urges re-evaluation of the Fenton(-like) system for sludge dewatering, given that Cu 3+ could also cause potential oxidative destruction of EPS compared with reactive oxygen species.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 14
·40534-40550
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IF 5.8
Fang Lei,Wu Guojian,Yao Keyu,Zhang Dongyang,Zhou Yongchao
A novel heterogeneous catalyst named MoS 2 /MIL-53(Fe, Cu) (MMFC) was prepared by hydrothermal method and applied in a heterogeneous electro-Fenton (hetero-EF) system for lomefloxacin (LOM) degradation in this work. Under the optimal conditions of current density 3 mA/cm 2 , catalyst dosage 0.100 g/L, and initial pH 6, 93.5% LOM (2 mg/L) removal efficiency was achieved in the MMFC hetero-EF system within 60 min, indicating an obvious improvement compared with the MIL-53(Fe, Cu) hetero-EF system. The good catalytic activity was attributed to more effective active sites of the catalyst and the conversion of Fe(II)/Fe(III) and Cu(I)/Cu(II) promoted by Mo(IV) in MoS 2 , which could be inferred by scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS) characterizations. The reusability and stability of MMFC were explored based on five cyclic experiments, and the average degradation efficiency reached 73.9%. Furthermore, the hetero-EF system could achieve the total removal of moxifloxacin and tetracycline within 6 min and 40 min, respectively. Quenching experiments revealed that the hydroxyl radicals (·OH) were the main reactive radicals while superoxide radicals (·O 2 − ) and singlet oxygen ( 1 O 2 ) played a certain part in LOM degradation. Finally, the possible mechanism of the hetero-EF process and LOM degradation pathways were proposed, including substitution, elimination, and cleavage of ring structures. Accounting for good catalytic performance, low preparation cost, and satisfactory versatility, the MMFC exhibited good potential to work as a hetero-EF catalyst for wastewater treatment.
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FUEL
·
2023
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IF 7.4
Juan Li,Xiaolei Jiang,Mingyuan Zhu,Bin Dai
Oxidative desulfurization (ODS) is a promising technique for obtaining clean fuel. Designing and researching zirconium-based metal–organic frameworks (Zr-MOFs) with bimetallic catalytic sites are encouraging for its further development. In this study, Cu(Ⅰ)-MOF-808 was successfully synthesized through anchoring Cu + in MOF-808. Pyridine infrared spectrum (Py-IR) and NH 3 temperature programmed desorption (NH 3 -TPD) confirmed that Lewis (L) acid sites existed in the synthesized material. Cu(Ⅰ)-MOF-808 was applied into the ODS reaction, during the reaction process, L acid sites adsorbed sulfide, Cu + sustainably provided electron to H 2 O 2 to formed into •OH, with the synergistic effect of L acid sites and Cu + , 99.9 % of the dibenzothiophene was oxidated to dibenzothiophene sulfone in 120 min. In addition, the cyclic experiment indicated that the ODS performance of Cu(Ⅰ)-MOF-808 was maintained at 99.2 % after 12 times recycling. Powder X-ray diffraction (PXRD) spectra indicated the framework structure of the reused catalyst was stable, inductively coupled plasma optical emission spectrometer (ICP-OES) result displayed no metal ions (Zr, Cu) leaching after the ODS reaction, which also proved the catalytic stability of the Cu(Ⅰ)-MOF-808.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Guiming Xie,Rongrong Jin,Pengju Ren,Yunming Fang,Runduo Zhang,Zhou-jun Wang
Boosted CO 2 hydrogenation to methanol was achieved by introducing appropriate amount of Au into conventional Cu-based catalysts. The Au x Cu/ZnO bimetallic catalysts with various Au/Cu molar ratio (x = 0.001, 0.005, 0.02 and 0.05) were prepared by the co-precipitation method, among which the Au 0.005 Cu/ZnO catalyst exhibited the highest methanol production rate. The formation of Au-Cu alloy was identified on the Au x Cu/ZnO bimetallic catalysts. Experimental characterizations and density functional theory (DFT) calculations suggested metal-oxide interfaces with oxygen vacancies as intrinsic active sties for both un-promoted and Au-promoted Cu/ZnO catalysts. The promotion effect of Au in bimetallic catalysts was correlated with the increase of active sites, facilitation of CO 2 activation and modification of intermediate adsorption. The present work for the first time develops a promising Au 0.005 Cu/ZnO bimetallic catalyst with trace amount of Au (only 0.4 wt%) and provides insight into the reaction mechanism over Au-promoted Cu/ZnO catalysts for methanol synthesis via CO 2 hydrogenation.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Xin Fang,Ling Tan,Haopeng Luo,Fang Jiang,Huan Chen
Designing electrocatalysts for nitrate (NO 3 - ) reduction with excellent activity, low cost and stability is of great interest. Herein we synthesized a novel transition bimetallic phosphide (CuFeP-x, x referred to the phosphidation temperature) catalyst by phosphidation using CuFe-Prussian blue analogue (PBA) nanoparticles as the precursor. The obtained CuFeP-450 maintained the morphology of nanocube with the average size of 33.0 nm and bimetallic phosphide nanoparticles formed during the phosphidation process. The higher electrocatalytic activity of CuFeP-x in electrochemical NO 3 - reduction were attained as compared to that of calcined CuFe-450, because the CuFeP-x have a lower interface impedance and the dominated species for NO 3 - reduction changes from electron to atomic H* , which effectively enhanced the removal rate. The appropriate phosphidation temperature can form a crystal structure that facilitated reaction kinetics. As a result, CuFeP-450 showed the best electrocatalytic performance for NO 3 - reduction (99.42%), and the selectivity of N 2 can reach nearly 100% under the condition of 1000 mg L −1 chloride ions . This simple method using PBA with binary transition metals to prepare bimetallic phosphide provides a new direction for designing efficient non-noble metal electrocatalysts for NO 3 - reduction.
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