Journal of Energy Chemistry
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2023
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IF 13.1
Di Liu,Zhejiaji Zhu,Jiani Li,Li-Wei Chen,Hui-Zi Huang,Xiao-Ting Jing,An-Xiang Yin
The application of direct ethanol fuel cell (DEFC) has been bottlenecked by the sluggish ethanol oxidation reaction (EOR). Efficient electrocatalysts for the C−C bond cleavage are essential to promote EOR with high efficiency and C1 selectivity. Here, we prepared Rh–Cu alloy nano-dendrites (RhCu NDs) with abundant surface steps through controlled co-reduction, which exhibited significantly enhanced activity and C1 selectivity (0.47 mA cm −2 (ECSA) , 472.4 mA mg Rh −1 , and 38.9%) than Rh NDs (0.32 mA cm −2 (ECSA) , 322.1 mA mg Rh −1 , and 21.4%) and commercially available Rh/C (0.18 mA cm −2 (ECSA) , 265.4 mA mg Rh −1 , and 14.9%). Theoretical calculations and CO-stripping experiments revealed that alloying with Cu could modulate the surface electronic structures of Rh to resist CO-poisoning while strengthening ethanol adsorption. In situ Fourier transform infrared spectroscopy (FTIR) indicated that the surface steps on RhCu NDs further promoted the C−C bond cleavage to increase the C1 selectivity. Therefore, optimizing the surface geometric and electronic structures of nanocrystals by rational composition and morphology control can provide a promising strategy for developing practical DEFC devices.
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Journal of Physical Chemistry C
·
2023
·
IF 3.7
Minglu Li,Siyu Kuang,Hai Liu,Qun Fan,Sheng Zhang,Xinbin Ma
Significant efforts have been devoted to the investigation of catalysts for converting CO2 into C2+ products. Cu catalysts are attractive for their initial selectivities but limited by the low stability over time. Herein we investigated the stability of Cu catalysts in an operating CO2RR environment. Hydroxides in electrolytes were found to play a key role in morphology evolution of Cu catalysts and thus result in decreasing Faradaic efficiencies of C2+ products. To this end, we deposited a porous carbon overlay on Cu catalysts through a thermal annealing method. Physical characterizations and electrochemical measurements showed that the morphology of Cu catalysts and Faradaic efficiencies of products were well maintained during the reaction. As evidenced by Fourier transform infrared spectroscopy with phenolphthalein as a probe, the added carbon overlay could effectively resist the influence of hydroxide corrosion on Cu catalysts. This study provides an efficient strategy to improve the stability of copper catalysts toward electrochemical CO2 reduction.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Erjian Huang,Yueyang Xu,Yachun Ren,Peng Zhang,Yongping Zeng
Faujasite (FAU)-type zeolites are promising adsorbents for the removal of sulfides from fuels, but their micropores are not capable to accommodate the large-sized thiophenic compounds. FAU zeolites (NaX and NaY with the low and high Si:Al ratios, respectively) with hierarchical micro/mesoporous structures were synthesized by sequential acid-base treatment to enhance the adsorption capacity and reduce the limitations of diffusion for the sulfides. To further to improve the desulfurization performance, the hierarchical structure of FAU zeolites containing Cu + were prepared by ion-exchange and methanol vapor-induced reduction methods at a relatively low temperature (473 K). For the large-sized benzothiophene , both the HP-Cu(I)Y and HP-Cu(I)X zeolites with mesopores have a very high adsorption capacity, reaching 51.8 mg S/g and 56.1 mg S/g, respectively. In addition, the results show that HP-Cu(I)X has a higher adsorption capacity than that of some other FAU-type adsorbents reported.
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Journal of Energy Chemistry
·
2022
·
IF 13.599
Huan Xie,Ruikuan Xie,Zhiyuan Zhang,Yongyu Pang,Yuting Luo,Jiong Li,Bilu Liu,Maria-Magdalena Titirici,Guoliang Chai
The conversion of CO 2 into value-added chemicals coupled with the storage of intermittent renewable electricity is attractive. CuO nanosheets with an average size and thickness of ∼ 30 and ∼ 20 nm have been developed, which are in situ reduced into Cu nanosheets during electrochemical CO 2 reduction reaction (ECO 2 RR). The derived Cu nanosheets demonstrate much higher selectivity for C 2 H 4 production than commercial CuO derived Cu powder, with an optimum Faradaic efficiency of 56.2% and a partial current density of C 2 H 4 as large as 171.0 mA cm −2 in a gas diffusion flow cell. The operando attenuated total reflectance-Fourier transform infrared spectra measurements and density functional theory simulations illustrate that the high activity and selectivity of Cu nanosheets originate from the edge sites on Cu nanosheets with a coordinate number around 5 (4–6), which facilitates the formation of *CHO rather than *COH intermediate, meanwhile boosting the C C coupling reaction of *CO and *CHO intermediates, which are the critical steps for C 2 H 4 formation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Ting Wang,Fuli Sun,Shoujie Liu,Guilin Zhuang,Benxia Li
Supported Cu single-atom (Cu-SA) catalysts have exhibited unique activity and selectivity in CO 2 reduction, but they generally suffer from the easy transformation of active Cu δ+ into inactive Cu 0 . Herein, porous TiO 2 supported Cu single atoms (Cu-SAs/TiO 2 ) photocatalyst was fabricated and dioxygen (O 2 ) enhanced photocatalytic CO 2 reduction performance of Cu-SAs/TiO 2 was investigated by in-situ characterizations and theoretical calculations. The results showed that both activity and stability of Cu-SAs/TiO 2 photocatalyst could be improved by feeding a small amount of O 2 (117.6 ppm) in the reaction system. The competitive electron transfer to O 2 on Cu-SAs/TiO 2 maintained dynamic stability of Cu δ+ active sites, and O 2 -derived *OOH species lowered the formation energy barrier of key intermediate *COOH as well as delivered *H species for accelerating intermediates protonation process. Total yield rate of CH 4 and CO reached 34.64 μmol·g cat ·h −1 for CO 2 photoreduction over Cu-SAs/TiO 2 after introducing 117.6 ppm O 2 , accompanied by enhanced durability.
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SENSORS
·
2023
·Vol. 23
·期 2
·695
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IF 3.9
Zhipeng Yu,Huan Wu,Zhongshuang Xu,Zhimao Yang,Jian Lv,Chuncai Kong
Designing highly active material to fabricate a high-performance noninvasive wearable glucose sensor was of great importance for diabetes monitoring. In this work, we developed CuxO nanoflakes (NFs)/Cu nanoparticles (NPs) nanocomposites to serve as the sensing materials for noninvasive sweat-based wearable glucose sensors. We involve CuCl2to enhance the oxidation of Cu NPs to generate Cu2O/CuO NFs on the surface. Due to more active sites endowed by the CuxO NFs, the as-prepared sample exhibited high sensitivity (779 μA mM−1cm−2) for noninvasive wearable sweat sensing. Combined with a low detection limit (79.1 nM), high selectivity and the durability of bending and twisting, the CuxO NFs/Cu NPs-based sensor can detect the glucose level change of sweat in daily life. Such a high-performance wearable sensor fabricated by a convenient method provides a facile way to design copper oxide nanomaterials for noninvasive wearable glucose sensors.Keywords:noninvasive wearable sensing;metal oxide;sweat glucose detection
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Chang Xu,Yue Feng,Xin-Xin Zhao,Shan Zhao,Shu-Guang Wang,Chao Song
Tetracycline (TC) and Cu(II) have been frequently detected in natural and engineering waters, especially in aquaculture water. However, literatures involving in the influence of Cu(II) on the transformation of TC are still insufficient. In this study, we investigated the photolytic fate of TC induced by Cu(II) under UV irradiation. Cu(II) significantly promoted the removal of TC with photolysis rate constant of 0.467 h −1 at TC:Cu(II) molar ratio = 1, which was 49.04% higher than that without Cu(II) (0.238 h −1 ). Cu(II) exhibited multiple influences on both direct and indirect photolysis of TC. Singlet oxygen ( 1 O 2 ) and hydroxyl radicals (·OH) made a major contribution to Cu(II)-induced TC photolysis, with contribution rates of 24.69% and 12.96%, respectively. Besides, Cu(II) preferred to complex between O20-O21 or O26-O27 to form TC-Cu(II) complexes with complexation ratio of 1. The Condensed Fukui Function and Condensed Double Descriptors values of TC-Cu(II) complexes were calculated for the first time with density functional theory. It showed that TC-Cu(II) complexes were more vulnerable to ROS attack, thus promoting TC degradation. Moreover, Cu(II) greatly changed the photolysis path of TC, mainly through hydroxylation, hydrogen extraction, and deamidation reaction into new byproducts. Furthermore, Cu(II) changed the toxicity of the products via changing the original TC photolysis products. This study provides new insights for the environmental fate of antibiotics, and also has far-reaching implications for wastewater treatment in pharmaceutical and aquaculture industry.
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MOLECULES
·
2023
·Vol. 28
·期 16
·5988
·
IF 4.6
Li Fan,Hongliang Zhu,Kaili Wang,Hao Liu,Weina Hu,Xin Xu,Shancheng Yan
Treatment of organic wastewater is still a difficult problem to solve. In this paper, Cu-doped SnSe powder was synthesized by a convenient and efficient hydrothermal method. Meanwhile, the degradation effect of different doping concentrations of SnSe on methylene blue was investigated. It was found that at low doping concentrations, the degradation effect on methylene blue was not obvious because Cu was dissolved in the lattice of the SnSe matrix at low concentrations. As the doping concentration increased, SnSe changed from a layered structure to a nanocluster structure with reduced particle size, and a mixed phase of SnSe and Cu2SnSe4appeared. In fact, the degradation effect on methylene blue was significantly enhanced, and we found that the catalytic degradation effect on methylene blue was best at a doping concentration of 10 wt.%.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Jinglin Zhu,Yutao Huang,Juanjuan Peng,Shaomin Liu
Developing simple and effective activation approaches to degrade phosphonate is crucial due to its potential aquatic environmental risks. Recently, Cu(II)-mediated activation processes provide a feasible method via nonradical oxidation mechanism to remove phosphonate, but is yet challenged under neutral conditions. Herein, a strategy for enhancing the Cu(II)/peroxymonosulfate (PMS) process by adding hydroxylamine (HA) could efficiently degrade 1-hydroxyethane1,1-diphosphonic acid (HEDP) at pH = 7.0. After 15-min reaction, 85.7% of total phosphorus (TP) in HEDP transformed into PO 4 3− in the Cu(II)/PMS/HA process is observed, which is 3.4 times than that in the Cu(II)/PMS process. The results of multiple experiments confirm that the presence of HA accelerates the reduction of Cu(II) and the generation of reactive species, SO 4 •− and Cu(III) induced intramolecular electron transfer as the primary reactive species play a significant role in the degradation of HEDP. Additionally, the removal of HEDP is inhibited with the addition of Cl − and HCO 3 − in the Cu(II)/PMS/HA process. However, the Cu(II)/PMS/HA process demonstrates a superior removal effectiveness of HEDP in different actual wastewater samples compared to the Cu(II)/PMS process under neutral conditions. This study provides an effective method for removing phosphonate from actual wastewater.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 36
·16864-16871
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IF 3.3
Lingling Lv,Yaoqing Chu,Lianjiang Tan
Antibacterial RBS@Cu:ZnO nanoparticles (NPs) were prepared by decorating Cu-doped ZnO NPs with Roussin's black salt (RBS), a nitric oxide (NO) precursor. Transmission electron microscopy (TEM) and dynamic light scattering (DLS) tests indicated that the RBS@Cu:ZnO NPs were particulate matter with crystal morphology and nanoscaled sizes. X-ray diffraction (XRD) patterns revealed the wurtzite crystal structure of the NPs. Under irradiation of 543 nm laser, the RBS@Cu:ZnO NPs released NO in a controllable manner due to the decomposition of RBS. Cu-doped ZnO with a Cu/Zn molar ratio of 5% showed antibacterial activity in response to ultraviolet and visible light by photocatalysis. The doping of Cu enhanced the visible light absorption of ZnO by reducing its band gap. The RBS@Cu:ZnO NPs exhibited high antibacterial activity originating from the synergistic bacterial inhibitory effects of Cu-doped ZnO and released NO under visible laser irradiation. More importantly, the antibacterial activity could be controlled by adjusting the power output of laser irradiation. The RBS@Cu:ZnO NPs are promising antibacterial agents with potential applications in biomedicine and pharmaceutics.
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JOURNAL OF DRUG TARGETING
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2022
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IF 5.016
Rui Kang,Mengdi Song,Zhou Fang,Kehai Liu
Vasculogenic mimicry (VM) describes the phenomenon whereby fluid-conducting vessels are formed by highly invasive tumour cells, which supply blood to tumours during their early growth stages. Single antiangiogenic agents have limited inhibitory effects on VM, therefore, a multi-pathway anti-VM strategy is required. In this study, Apatinib (Apa) was coordinated with Cu2+ to form a Cu-Apa copper complex. The latter was loaded into oligo-hyaluronic acid (HA) polymeric micelles (HA-Chol) and subsequently embedded in Astragalus polysaccharide-based in situ hydrogels (APsGels) to generate Cu-Apa/HA-Chol@APsGels. In this system, Cu-Apa exerts the combined effects of Cu2+ and Apa to inhibit VM; HA-Chol micelles achieve targeted drug delivery and enhance endocytosis efficiency; APsGels realise sustained release of the drugs to ensure an anti-VM effect. This system demonstrated improved VM inhibition with low cytotoxicity and high biocompatibility, wound healing, and transwell invasion in three-dimensional cell cultured VM. Moreover, this system significantly inhibited VM formation and melanoma growth in a mouse tumour transplantation model. This study provides an effective strategy for inhibiting VM.
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Journal of Materials Chemistry C
·
2022
·Vol. 10
·期 35
·12602-12609
·
IF 8.067
Chen Jia,Hongli Liu,Xiaoyuan Zhang,Shirong Wang,Xianggao Li
Self-powered photodetectors are great potential candidates in the next generation of low energy-consumption photoelectric devices. However, the planar-type metal–semiconductor–metal (MSM) self-powered photodetectors (PDs) of perovskites still suffer from poor photodetection performance. Herein, by taking advantage of the spontaneous polarization property of the CH3NH3PbI3 single crystal, which can generate an extra polarization electric field, planar-type self-powered Au/CH3NH3PbI3/Cu PDs with preferable photodetection capability is reported. The resultant PDs exhibit the maximum responsivity of 0.288 A W−1 in 400–840 nm under the superposed built-in electric field by spontaneous polarization and asymmetric Schottky junction. Furthermore, the maximum detectivity is 4.69 × 1012 Jones, which is the highest record among the planar-type MSM self-powered PDs based on a perovskite. Moreover, the PDs exhibited excellent operation stability with the photocurrent of the unencapsulated photodetector remaining at 92% after 15 days in atmospheric condition.
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