AICHE JOURNAL
·
2025
·
IF 4
Hui Wang,Yifan Jin,Yaxin Jin,Siyu Kuang,Tianxiang Yan,Xinyue Wang,Xiao Wang,Wenquan Cui,Sheng Zhang
Electrochemical carbon dioxide reduction reaction (CO 2 RR) is one of the most prospective strategies to achieve carbon neutrality. Multi-carbon compound (C 2+ ) products have higher commercial value and wider applications, among which ethanol is a widely used chemical feedstock and high energy density fuel. Here, we prepared nitrogen-doped carbon nanofibers containing copper-zinc double atoms using the electrospinning technique and controlled the content of both metal atoms by varying the calcination temperature. This catalyst exhibited ultra-high selectivity for ethanol at low potentials. Ethanol selectivity at −0.3 V versus RHE was more than 60% with the total alcohol selectivity of over 80%. Meanwhile, we explored the ethanol production pathway by combining density-functional theory (DFT) and ATR-FTIR spectroscopy, and found that OCCO* intermediates were most abundant for the optimal ratio of Cu to Zn atoms, lowering the energetic barriers to ethanol formation, and thus improving the selectivity of ethanol production.
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CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Yi Fang,Lang Yang,Feng Rao,Yongming Zheng,Zhenguo Song
In this study, a low-cost porous geopolymers (PGP) were prepared using coal gangue and fly ash as raw materials to remove organic and heavy metal ions from wastewater. Various characterization techniques were employed to investigate the microstructure, morphology, pore size distribution, and surface functional groups of the porous geopolymers. The results indicate that the geopolymer exhibits a porous structure with hydroxyl groups on the surface after foaming. It was found that the porous geopolymers exhibited good adsorption capacity for Methylene Blue (MB), Cu(II), and Pb(II), with optimal adsorption capacities reaching 35.60 mg/g, 98.31 mg/g, and 85.67 mg/g, respectively. Fitting analysis suggests that the adsorption of MB, Cu(II), and Pb(II) is better described by the pseudo-second-order kinetic model and the Freundlich isotherm model. This indicates that the adsorption process is primarily chemical adsorption with multilayer adsorption. Competitive adsorption studies showed that Cu(II) could enhance the adsorption of MB, while Pb(II) had no significant effect on the adsorption of MB. Mechanistic studies revealed that the adsorption of MB by PGP is mainly through pore adsorption, electrostatic attraction, and hydrogen bond formation; whereas the adsorption of Cu(II) and Pb(II) is primarily through pore adsorption, electrostatic attraction, chemical reactions, and ion exchange. Recycling experiments demonstrated that after five repetitions, the adsorption capacity of PGP for the three pollutants remained above 60 %. These findings confirm the potential of porous geopolymers as adsorbents. Preliminary cost analysis shows that the adsorption cost of porous geopolymers is only 2.07 RMB/kg, making the geopolymer adsorbent economically advantageous and promising for application, especially considering its ability to utilize industrial solid waste.
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FUEL
·
2024
·
IF 6.7
Jingjing Wang,Xinjie Wei,Zhihui Wen,Junjie Liao,Liping Chang,Jiancheng Wang,Kechang Xie
Ultra-deep desulfurization for the generation of clean petrol, diesel, and benzene remains a significant and challenging goal globally. Cu-containing materials have emerged as a promising desulfurization strategy due to their high adsorption capabilities. However, existing reduction technologies often lead to over-reduction. In this study, we reveal an intriguing and unexpected property of Y zeolite following ammonium ion exchange. The in situ generation of ammonia from ammonia pools may alter the location of copper species and modify their acid characteristics. We encapsulated various amounts of Cu into CuY zeolite, labelled as H-Cu X -Y(APE), using a facile self-reduction strategy. Notably, H-Cu 5.71 -Y(APE) exhibits an exceptional breakthrough sulfur capacity for thiophene, achieving 4.17 mg/g, nearly double that of traditional Cu-HY(H 2 ). XPS analysis following APE reduction indicates a high proportion of Cu + species in H-Cu 5.71 -Y(APE). In situ calcination FT-IR provided detailed insights into the chemical transformation of Cu 2+ species during APE reduction. Furthermore, CO-FTIR analysis shows that the Cu + content in the supercages of H-Cu 5.71 -Y(APE) reaches a maximum of 62.3 %. Py-FT-IR reveals the strong Brønsted acid content in H-Cu X -Y(APE) significantly increases. The desulfurization mechanism of H-Cu X -Y(APE) was thoroughly investigated using in situ FT-IR, demonstrating that the protonation and copolymerization of thiophene occurred on HCuY(APE) and could be effectively suppressed by adjusting the amount of copper. This work presents a promising solution for efficient ultra-deep desulfurization using an in situ NH 3 reduction method from ammonia pools.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Tianyun Jing,Shaokang Yang,Tingting Li,Yangyang Wan,Huimin Jia,Yonghai Feng,Yunpeng Zuo,Dewei Rao
Atomic scaling of cobalt-based catalysts is the feasible and sustainable approach for selective oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to produce bio-plastic monomer of 2,5-furandicarboxylic acid (FDCA) under mild conditions. Here, a high-efficiency dual single-atomic Co/Cu supported on nitrogen-doped carbon (a-Co/Cu-NC) is constructed. Leveraging exceptional oxygen activation ability, the Co/Cu dual-atomic-sites can accelerate the HMF oxidation, suppressing by-product formation mediated by reactive oxygen species (ROS) in low-oxygen environments. This leads to enhanced FDCA selectivity with a yield of 98% and a production rate of 298.8 mmol FDCA g metal −1 h −1 under ambient conditions. Comprehensive experiments and density functional theory (DFT) calculations demonstrate that long-range interactions between Co and Cu sites optimize reactant adsorption and lower energy barriers for •O 2 − and HMFCA formation.
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Scientific Reports
·
2017
·Vol. 7
·期 1
·1-13
·
IF 4.259
Wang Xiaoxia,Zhang Baoqin,Zhang Wei,Yu Mingxun,Cui Liang,Cao Xueying,Liu Jingquan
Graphene oxide (GO) was rarely used as microwave absorption (MA) material due to its lower dielectric loss compared with reduced GO (RGO). However, the characteristics of low conductivity, light weight, and large surface area were beneficial to the impedance matching for absorbers already containing highly conductive metal materials. Cu@Ni nanowires are promising MA materials due to the desired dielectric loss from copper and excellent magnetic loss from nickel. However, the high density was an impediment to its further application. Combining Cu@Ni nanowires with GO should be an effective solution to decrease the absorber’s density and improve its MA properties. Herein, we demonstrated that Cu@Ni nanowires/GO composites exhibited enhanced MA capacities compared with Cu@Ni nanowires or GO alone, and the minimum reflection loss reached −42.8 dB at 16.9 GHz with a thickness of 2.1 mm. The enhanced MA performance mainly originated from good impedance matching, as a result of the addition of low conductivity of GO. To confirm this point, the MA performance of Cu@Ni nanowires/RGO was studied, and unsurprisingly, weak MA performance was obtained. Our work provides a new strategy to decrease the density, broaden the frequency band and tune MA performance of composites.
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高影响因子
Materials Today Sustainability
·
2024
·
IF 7.1
Guilu Qin,Yifan Liu,Ruhumuriza Jonathan,Baoshan Wu,Xian Jian
TiO 2 semiconductor has the disadvantages of energy bandwidth, low photo-quantum efficiency, and electron-hole pair easy recombination, which makes TiO 2 semiconductor photocatalytic materials cannot be widely used efficiently. Here, a simple and low-cost method is used to prepare TiO 2 /C/Cu hybrid by in-situ carbon reduction by chemical vapor deposition. During high-temperature calcination, an amorphous carbon is formed on the surface of anatase TiO 2 , and CuO is reduced by in-situ carbon to obtain Cu. Partial Cu-doping into TiO 2 introduces defects, and in-situ Cu and C loads act as electron traps to reduce photogenerated electron/hole recombination. Compared with the original TiO 2 , the TiO 2 /C/Cu hybrids have a narrow band gap (2.77 eV) and abundant defect active sites and have excellent photocatalytic activity to improve the degradation of formaldehyde (HCHO) and methyl orange (MO) under visible light. In addition, after 4 cycles, the degradation of HCHO and MO still maintained excellent stability. This innovation has many potential applications in the future, including air purification and industry.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Ling Zhou,Yaoyu Zhang,Yue Liu,Zhongbiao Wu
This work investigated the reaction behaviors of diethylamine (DEA) catalytic oxidation on various Cu-based catalysts with different supports (TiO 2 , HZSM-5(27), HZSM-5(130) and S-1). It was found that the acidic environment of catalysts greatly influenced reaction pathways of DEA oxidation. On Cu 5 /TiO 2 catalyst mainly with Lewis acidity, DEA preferentially dissociated through a two-step dehydrogenation to produce acetonitrile and ethylene, while on Cu 5 /HZSM-5(27) catalyst with strong Brønsted acidity, DEA could directly decompose into ethylamine and ethylene via N-C cleavage. Both pathways existed simultaneously over Cu 5 /HZSM-5(130) with decreased Brønsted acidity. Thereafter, acetonitrile could be further oxidized on the Cu 5 /TiO 2 catalyst to generate a large amount of NO x via NCO(a) intermediates over-oxidation, while ethylamine on Cu 5 /HZSM-5 samples would convert to acetamide and then produced N 2 and CO 2 . The Cu 2+ species due to enriched Brønsted acid sites in Cu 5 /HZSM-5 catalysts ensured excellent N 2 selectivity via internal SCR mechanism. Additionally, the strong Brønsted acidity of Cu 5 /HZSM-5(27) could induce the polymerization of carbonaceous intermediates and thereby resulted in severe coke deposition. As for Cu 5 /HZSM-5(130) and Cu 5 /S-1 with relatively lower Brønsted acidity and reducibility would release some unwanted gas-phase by-products like ethyl-isocyanate. This work provided useful guidance for designing NVOCs catalysts with high activity and less toxic by-products.
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Chemical Engineering and Processing-Process Intensification
·
2024
·
IF 3.8
Xiaocui Zhang,Xiaoxin Wang,Jun Gao,Jiangcheng Li,Xiangfeng Liang,Qinghui Shou
The global need for bromide ions (Br - ) has driven the research focus to extract them from various liquid ores. Highly efficient and selective adsorbent is still lacking. MOF with large surface area and structural stability are promising candidate for Br - extraction. In this work, we prepared Cu-MOF-74 nanocrystals. Abundant hydroxyl groups on them spontaneously reduced Ag + to Ag 0 nanoparticles, resulting in the fabrication of Ag 0 doped Cu-MOF-74. The crystalline structure retains after the doping of Ag 0 when the mass ratio of silver nitrate to MOF is <0.5. The crystals are distorted or even damaged when the ratio is higher than 1.0 according to XRD and DFT calculation. The adsorption capacity of Ag 3 -Cu-MOF-74 is 232.92 mg g -1 , surpassing the capacities of most previously documented adsorbents. The desorption of Br - and thereafter the recovery of adsorbent could be realized through light driven decomposition of AgBr. This MOF adsorbent shows promising application potential in Br - recovery from various liquid ores.
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Advanced Healthcare Materials
·
2025
·
IF 9.6
Xianyu Zhu,Lingli Gao,Yanbo Zheng,Peng Fei Zhao,Hanrui Wei,Ruixue Liu,Liping Zhao,Junyi Zhang,Qi Sun,Lingling Zheng,Han Lv,JiGang Yang,Jianhua Gong,Zhenchang Wang
Poor prognosis and chemotherapy response stem from difficulties in precise targeting and the lack of effective synergistic treatments. Nanozymes show promising potential in tumor chemodynamic therapy (CDT) by catalyzing hydrogen peroxide (H₂O₂) decomposition and glutathione depletion in the tumor microenvironment (TME). However, integrating precise chemotherapy targeting with CDT remains challenging. In this study, a porous Fe/Cu bimetallic nanozyme carrier (FeCuNPs) is developed for co-loading with the humanized 3F8 anti-GD2 disialoganglioside antibody (3F8) and the novel pyridazinone-based chemotherapeutic agent (IMB), forming a nanoreactor (3F8@FeCuNPs@IMB) for targeted chemotherapy and CDT. The nanoreactor responds specifically to the acidic TME as a primary insurance, allowing for the controlled release of IMB at the tumor site. The targeting antibody 3F8 coating on the surface of the nanozyme carrier acts as a secondary insurance, minimizing chemotherapy drug leakage during the delivery process and ensuring precise targeting for effective chemotherapy. Furthermore, FeCuNPs act as peroxidase-like (POD) and glutathione oxidase-like (GSHOX) enzymes, catalyzing hydroxyl radical (•OH) generation and depleting excess GSH, enhancing CDT. The results in vitro and in vivo indicate that the dual insurance designed 3F8@FeCuNPs@IMB offers a promising prospect for a targeted, precise, and effective combination of chemotherapy and CDT against melanoma.
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高影响因子
RSC Advances
·
2024
·Vol. 14
·期 48
·35993-36004
·
IF 3.9
Jinlong Zhong,Xue feng Mao,Guanyu Wang,Heng Li,Junfang Li,Sijian Qu,Jianwei Zhao
Non-homogeneous ozone-catalyzed oxidation technology is one of the effective ways of treating wastewater, the core of which lies in the development of efficient ozone oxidation catalysts. This work proposes the design and synthesis of an efficient Cu/Mn/Ce multi-metal composite oxide catalyst by metal salt precursor mixing-direct granulation. The effect of metal doping on the catalyst properties was compared using Density function theory (DFT) calculations, and the Cu/Mn/Ce co-doping showed significant charge accumulation effect with a low ozonolysis energy barrier, which is more favorable for the generation of reactive oxygen species. The successful loading of the main active metal components, such as Mn, Cu, and Ce, was clarified by systematic characterization by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS) and Brunauer–Emmett–Teller's test (BET), and the chemical oxygen demand (COD) removal could reach more than 60% for the simulated wastewater. The electron paramagnetic resonance (EPR) characterization clarified that the degradation of organic pollutants was mainly dominated by the combination of single-linear oxygen and superoxide radicals in the catalytic process, and the possible catalytic oxidation mechanism was proposed. This work advances the development of non-homogeneous ozone oxidation technology.
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高影响因子
RARE METALS
·
2024
·
IF 9.6
Feng Yu-Xiao,Yu Hui-Jun,Lu Tian-Guang,Zheng Zi-Ye,Tian Shuang,Xiang Li,Zhao Shan,Wang Shu-Guang,He Zuo-Li
Metal clusters or even single-atoms dispersed and anchored on the photocatalysts’ surface can enhance photocatalytic performances on organic pollutant oxidation. Here, a simple photoreduction method was used to create atomically dispersed metal single-atoms/clusters (MSCs, M = Cu, Pd, Au and Ag) on P-modulated tubular carbon nitride (TCN). The obtained MSCs@TCN demonstrated excellent photocatalytic performances for the degradation of sulfamethazine (SMZ). In particular, the photocatalyst with 2 wt% Cu loading showed ultrahigh SMZ oxidation efficiency ( k = 0.06110 min −1 ), almost three times that of TCN ( k = 0.02066 min −1 ). It also shows excellent stability in the 5th-cycle measurements. The improved photocatalytic activity of the CuSCs@TCN is ascribed to the synergistic promotion of photogenerated charge separation by Cu single-atoms/clusters as active sites, accelerated charge transfer from bulk TCN to Cu sites through Cu–N x interaction. Meanwhile, the active sites of Cu single-atoms/clusters could promote the production of ·O 2 − , which participates in organic oxidation with strong oxidizing holes (h + ). This strategy paves a new avenue for designing high-performance photocatalysts decorated with metal single-atoms and clusters.
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Coatings
·
2024
·Vol. 14
·期 2
·164
·
IF 2.9
Wanlei Dai,Zhaoyi Jiang,Yali Sun,Juhua Wang,Zeran Gao,Haoyu Xu,Xinzhan Wang,Chao Gao,Qiang Ma,Yinglong Wang,Wei Yu
In this study, a feasible strategy is proposed for directly depositing high-quality Cu(In,Ga)Se2(CIGS) films using Na-doped targets in a selenium-free atmosphere to boost the power conversion efficiency (PCE) of CIGS solar cells. Introducing a small amount of sodium dopant effectively promoted the textured growth of CIGS crystals in the prepared films, resulting in larger grain sizes and a smoother interface. The higher MoSe2content at the CIGS/Mo interface increased the carrier lifetime in the films. In addition, sodium doping increased the proportion of Se atoms on the film surface and reduced the concentration of defects caused by the direct sputtering of the films in the selenium-free atmosphere. Therefore, the separation and transportation of photo-generated carriers in the devices were effectively enhanced. Using the optimized parameters, a record-high PCE of 17.26% was achieved for the 7.5% Na-doped devices, which represents an improvement of nearly 63%.Keywords:Cu(In,Ga)Se2;sodium-doped targets;magnetron sputtering;solar cells
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