JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yurui Xu,Xiao Liu,Minghui Jiang,Ning Li,Mingxue Su,Xin Du,Shiyu Li,Lei Lu,Suping Cui
Electrochemical carbon dioxide reduction reaction (ECO 2 RR) to produce high value-added products is a promising and effective strategy for closing the artificial carbon cycle and achieving sustainable development of resource. However, catalyst structural reorganization and agglomeration caused by the reduction process will reduce the catalytic performance. In this study, a carbon nitrogen shell with cupper-doped (CNCu shell) catalyst was prepared using silicon dioxide (SiO 2 ) as a template. The selectivity of the catalyst was controlled by precisely adjusting the form of Cu doping in the catalyst. When doped as single-atoms (CNCu 2.5 ), the catalyst exhibited a Faraday efficiency of up to 85 % for formate at −0.9 V versus reversible hydrogen electrode (vs. RHE). In contrast, when both Cu clusters and single-atoms coexisted (CNCu 25 ), the catalyst favored multi-carbon products, with a Faraday efficiency of 45 % for ethanol and 23 % for acetic acid. Density functional theory (DFT) calculations revealed the key mechanism for the difference in catalyst selectivity between the two doping forms. Cu single-atoms provided suitable binding energy to HCOO*, which increased the rate of CO 2 conversion to formate, while the combination of Cu clusters and single-atoms increased the adsorption of HCOO*, raising the rate-determining step energy of the formate pathway, which favored multi-carbon products. This study fundamentally revealed how different doping forms of metals affect catalyst selectivity, providing new insights and strategies for developing superior metal–carbon–nitrogen (M C N) catalysts.
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Journal of Water Process Engineering
·
2024
·
IF 6.3
Chuangbin Hong,Jiehang Zhou,Wenguang Wang,Liangpeng Wu,Shimin Long,Wentao Zhou,Yuxi Guo
Catalytic activation of peroxymonosulfate (PMS) is one of the important research areas in the development of advanced oxidation technology for wastewater treatment. At present, the development of high-performance catalysts for PMS activation has become a research hotspot. Herein, (Cu + decorated g-C 3 N 4 )/Bi 2 WO 6 ((Cu + /g-C 3 N 4 )/Bi 2 WO 6 ) composite was prepared successively by calcination and solvothermal method, which was used in visible light-assisted PMS activation for the degradation of rhodamine B (RhB). The construction of S-scheme heterojunctions between Cu + decorated g-C 3 N 4 and Bi 2 WO 6 facilitated the activation of PMS, leading to a RhB degradation ratio of 98.46 % within 50 min. The corresponding reaction kinetic was significantly improved by a factor of 2.32 and 7.94 compared with that of CCN and BWO, respectively. The enhanced performance of the (Cu + /g-C 3 N 4 )/Bi 2 WO 6 can be attributed to the successful construction of S-scheme heterojunction, which facilitates the separation of photogenerated carriers and accelerates the PMS activation to produce abundant active species. Furthermore, the (Cu + /g-C 3 N 4 )/Bi 2 WO 6 composites exhibit strong stability and reusability following three cycles. In addition, the intermediates produced during the RhB degradation process were investigated by liquid chromatograph mass spectrometer (LC-MS). This study provides a new insight into the preparation of S-scheme photocatalysts for the photocatalytic-PMS activation system that will achieve efficient removal of dyes from wastewater.
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ACS Catalysis
·
2025
·
IF 13.1
Ziyang Chen,Hua Tong,Yun Zhao,Jie Cui,Lei Zhou,Jiale Zou,Fuqiang Zhou,Peirong Chen,Daiqi Ye,Limin Chen
TiO2 as a reducible metal oxide has been extensively employed as a support for noble and transition metals. Numerous studies have demonstrated that optimizing metal–TiO2 interactions can significantly enhance the catalytic performance. Meanwhile, the weak metal–support interaction between Cu and TiO2 generally results in unsatisfactory catalytic performance for the hydrogenation of CO2 to methanol. Herein, through support facet and defect engineering, the electron transfer from TiO2 to Cu nanoparticles (NPs) is successfully constructed over Cu/TiO2 (001) catalysts, enabling a sharply enhanced methanol yield of about 7.2% at 5 MPa and 280 °C. Detailed characterizations reveal that the regulation of support defects and the catalyst preparation process boost the defect density over TiO2 and then facilitate the electron transfer from TiO2 to Cu NPs and the highly dispersed electron-rich Cu NPs. This, in turn, promotes the dissociation and spillover of H2, further producing support defects and achieving dynamic regulation. Ultimately, these synergistic interactions drive the hydrogenation of CO2 to methanol. These findings not only demonstrate the Cu/TiO2-based catalyst as one of the most promising catalysts for CO2 hydrogenation to methanol but also establish a generalizable strategy for enhancing catalytic performance through support facet and defect-engineered electron transfer modulation.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·
IF 2.7
Na Ma,Ke Li,Bo Xu,Huafeng Tian,Songbai Ma,Jinlong Li,Yuge Ouyang,Qian Liu,Dagang Liu,Rakesh Kumar
To solve the problem of the presence of heavy metals in water causing water pollution, the biodegradable film based on zein/polyvinyl alcohol (PVA) with the incorporation of nano-hydroxyapatite (nHAP) was fabricated through an electrospinning technique. The copper ion was taken as the representative of heavy metal ions in this study. The result showed that the incorporated nHAP nanoparticles were dispersed within the zein/PVA matrix, and strong hydrogen bonding interactions were formed between the filler and matrix, improving the hydrophobicity of the nanofibrous films and maintaining thermal stability. The adsorption mechanism was analyzed by fitting the adsorption process with pseudo-first-order model and pseudo-second-order model. Based on the ion exchange effect, electrostatic interaction, and complexation, the adsorption capacities of nanofibrous films for Cu(II) were significantly increased after adding nHAP. When the nHAP content was 20 wt.%, the Cu(II) adsorption capacity reached up to 23.86 mg/g, and the adsorption efficiency was 13.94% higher than that of neat zein/PVA nanofibers. This work suggests the potential of the electrospun zein/PVA/nHAP nanofibrous films as desirable eco-friendly materials in metal removal applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
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IF 20.2
Tianyi Wu,Jiaxuan Chen,Lingyue Liu,Xiaolei Qu,Shourong Zheng,Dongqiang Zhu
Electrochemical reduction of nitrate to ammonia (NH 3 ) provides an attractive approach to accomplish resource utilization of pollutants, while exploring efficient catalysts with high catalytic activity and NH 3 FE at low applied potentials remains great challenging. Herein, we constructed a three-dimensional Cu 3 P/Cu catalyst and studied its catalytic performances in electrochemical nitrate reduction reaction . The Cu 3 P/Cu catalyst with finely balanced metallic Cu and Cu 3 P sites exhibits a high NH 3 yield of 4.27 mg h −1 cm −2 after 1 h reaction at a low applied potential (-0.05 V vs RHE), outperforming most of previously reported Cu-based catalysts. DFT calculations demonstrate the favored reduction of nitrate to nitrite on metallic Cu and hydrogenation of nitrite to NH 3 on Cu 3 P. This study opens up new opportunities for the application of Cu 3 P/Cu catalyst as a robust tandem electrocatalyst in the large-scale production of NH 3 through electrochemical reduction with low energy consumption.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Kejing Wang,Yongjun Liu,Zhiwen Li,Nan Cui,Lei Sun,Wei Huang
The valence states of Cu site are regarded as an important factor affecting the performance of syngas to higher alcohols (C 2+ OH). Regrettably, the role of Cu 0 and Cu + in CO hydrogenation to higher alcohols remains controversial due to the complexity of the reaction. In this study, Cu 0 and Cu 2 O powders are directly added as the precursors to adjust the ratios of Cu + /(Cu 0 +Cu + ) and Cu particle sizes in CuZnAl catalysts by a complete liquid-phase (CLP) technology. The CAT-Cu 0 catalyst with higher Cu 0 content shows the highest CO conversion (>15%) ascribing to the biggest S Cu , but is also accompanied by the highest CO 2 selectivity (>40%), while the CAT-Cu + catalysts with higher Cu + content displays relative better C 2+ OH selectivity (>60%) and stability due to a higher probability of CO insertion. In-situ DRIFTS experiments reveal that a synergy between larger Cu particle sizes (30～40 nm) and surface Cu + sites, in which larger Cu sizes enhances the probability of bridge CO adsorption, thereby favoring the C–O bond dissociation for CH x formation. Meanwhile, Cu + active sites provide a higher probability for CO/CHO insertion to form CH 3 CHO*/CH 2 CO* intermediates. This study further deepens our understanding of the critical controlling factors for highly selective synthesis of C 2+ OH from syngas over Cu-based catalysts.
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APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Yue Li,Huan Ren,Daolai Sun,Xinqiang Zhao
Vapor-phase catalytic deoxydehydration of 1,2-propanediol (1,2-PDO) to form propylene was performed over various metal-loaded catalysts in an H 2 flow at an ambient pressure. Cu-based catalysts exhibited a relatively high activity for the formation of propylene, while other metal-based catalysts, such as Pt-, Ru-, Rh-, Ni-, and Co-loaded SiO 2 -Al 2 O 3 , primarily produced C-C bond cleavage products. Cu-loaded H 3 PO 4 /SiO 2 -Al 2 O 3 catalysts showed the best catalytic performance, and the catalyst with a Cu and H 3 PO 4 loading of 8 and 10 wt%, respectively, could provide a propylene selectivity of 95.0% with a complete conversion of 1,2-PDO at 280 °C. The Cu-loaded H 3 PO 4 /SiO 2 -Al 2 O 3 catalysts primarily contained Lewis acid sites, and the Cu particles were well dispersed on the catalyst surface with an averaged particle size of 3.1 nm. It is proposed that the vapor-phase deoxydehydration of 1,2-PDO to propylene undergoes multi-step reactions with propanal and 1-propanol as the reaction intermediates.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Man Dong,Qingqing Pan,Fanfei Meng,Xiaohui Yao,Siqi You,Guogang Shan,Chunyi Sun,Xinlong Wang,Zhongmin Su
Sunlight-driven CO 2 reduction to value-added chemicals is an effective strategy to promote carbon recycling. The exploration of catalysts with efficient charge separation is crucially important for highly efficient CO 2 photoreduction. In this work, the preparation of metal-cluster-based covalent organic framework (CuABD) integrated features from both metal organic frameworks (MOFs) and covalent organic frameworks (COFs) through the condensation of diamines and functionalized trinuclear copper clusters demonstrate a thoughtful design strategy. The reported yield of 1.3 mmol g −1 h −1 for formic acid (HCOOH) under simulated solar irradiation is impressive, surpassing the performance of many COF- and MOF-based catalysts previously reported. Compared to its isomorphic metal-free structure (named BDFTD) and bare trinuclear Cu cluster which present extremely poor catalytic activities, CuABD displays remarkably enhanced CO 2 reduction activity. Experimental and theoretical investigations reveal that the efficient charge transfer between diamine monomer and cyclic trinuclear copper (I) units, and the electron delocalization of the π-conjugated framework are responsible for the appealing catalytic performance. In summary, the work presents a well-structured and scientifically sound exploration of a metal-cluster-based covalent organic framework for efficient CO 2 reduction under sunlight.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2024
·
IF 3.2
Hongyan Zhang,Jiehui Huang,Yuxiang Shen,Zuofang Yao,Chenchen Xing,Yanping Hou
Z-Scheme heterojunction photocatalysts can effectively suppress the recombination of charge carriers while maintaining high redox capacity. In this study, ZnTe/WO 3 (ZW) Z-scheme heterojunction photocatalysts were synthesized using a hydrothermal method, and a series of photocatalytic materials were prepared for the simultaneous removal of tetracycline (TC) and Cu(II) from water. The physicochemical and photoelectrochemical properties of the catalytic materials were characterized through various methods, including SEM, XRD, XPS, and others. The experimental results indicate that the ZW-10 % composite material exhibits the most significant removal efficiency for pollutants. Within 150 min of visible light irradiation, the removal rates for TC and Cu(II) reach 73.8 % and 73.3 %, respectively, representing a substantial improvement compared to individual ZnTe and WO 3 . Free radical capture experiments and electron spin resonance analysis reveal that ·O 2 − and ·OH are the key reactive species responsible for TC oxidation, while electrons (e − ) dominate the reduction of Cu(II).
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Jieli Ou,Yiqing Liu,Linyue Zhang,Zhenran Wang,Yuqi Tang,Yongsheng Fu,Dandan Zhao
Although Cu(II)/peroxymonosulfate (PMS) process has been successfully applied to degrade varied organic contaminants in water, the slow transformation of Cu(II) to Cu(I) that works only in alkaline conditions retards the treatment efficiency of this process. In this study, a new finding was observed, that is, oxytetraczdycline (OTC) could effectively enhance the degradation of organic pollutants in Cu(II)/PMS process where it was also removed in acidic conditions. With the addition of OTC in Cu(II)/PMS system, 85.5% of rhodamine B (RhB) was degraded in 90 min at pH 4.0, which was far more than that without OTC (36.1%), and simultaneously 98.1% of OTC was eliminated. The added OTC could form OTC-Cu(II) complexes which might powerfully improve the reduction of Cu(II) to Cu(I), exerting a positive effect on the PMS activation and subsequent degradation of RhB. Electron paramagnetic resonance (EPR) experiments assisted with radical scavenging experiments and Raman spectrum detection results suggested that Cu(III) and hydroxyl radical (HO • ) were the predominant reactive species for RhB degradation, while OTC removal in this system was mainly ascribed to direct PMS oxidation. The Cu(II)/PMS process also showed a promising success on the synergistic degradation of OTC with the other four refractory organic pollutants , indicating the potential application of PMS oxidation in water treatment .
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FUEL
·
2024
·
IF 6.7
Ruhao Gong,Haihui Chen,Xiuya Rao,Jihong Chi,Ziqi Zhang,Guiling Xu,Dandan Chen,Qiang Zhou,Ping Lu
Mn/Cu co-doping mesoporous carbon sorbent (MnCu x -C) was synthesized via using hard template method. Thymol blue (C 27 H 30 O 5 S) was used as carbon source and MCM-41 was applied as template agent. Copper nitrate trihydrate (Cu(NO 3 ) 2 ·3H 2 O) and manganese acetate tetrahydrate (MnC 4 H 6 O 4 ·4H 2 O) was in-situ co-doped with carbon source as Cu/Mn metals precursor. Mercury removal on the MnCu x -C sorbent was investigated on a fixed bed experimental apparatus. The physical and chemical characteristics of the MnCu x -C sorbent were investigated by using BET, SEM, FTIR, XRD and XPS, respectively. Combing with mercury programmed temperature desorption (Hg-TPD) and density functional theory (DFT), the mechanism of mercury adsorption on the MnCu x -C sorbent was revealed. The results showed that the synthesized MnCu 0.1 -C sorbent displayed high mercury removal performance at 150℃, which was considered to be a potential sorbent for mercury removal from industrial flue gas. Mn doping on the mesoporous carbon greatly improved the mercury removal ability of sorbent with mercury capture rate increasing from 6 % to 89 %. Doping of Cu can effectively improve the SO 2 tolerance of the MnCu 0.1 -C sorbent for mercury removal. With different concentration of SO 2 existing in flue gas, the MnCu 0.1 -C sorbent still kept high mercury removal ability. O 2 in flue gas promoted mercury removal on the MnCu 0.1 -C sorbent with main product of HgO. In the presence of SO 2 , a small amount of HgSO 4 formed on the MnCu 0.1 -C sorbent. The DFT analysis further displayed that Hg 0 was mainly chemisorbed on the surface of MnCu 0.1 -C sorbent with formation of HgO.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2025
·Vol. 36
·期 19
·1-11
·
IF 2.8
Li Canglong,Wen Kexin,Zhang Bing,Chen Jie,Niu Xinshuai,Zou Boyuan,Lu Xuechi,Yang Wenqian
The structure, magnetic behavior and magnetocaloric performance in heavy rare–earth based compounds Tb 2 M TiO 6 ( M = Co, Ni, Cu) have been experimentally investigated in this work. The structural analysis indicates that Tb 2 CoTiO 6 and Tb 2 NiTiO 6 crystallize in a monoclinic double perovskite structure, while Tb 2 CuTiO 6 forms a hexagonal layered structure. The magnetic measurements reveal that the samples show high magnetic reversibility within a wide temperature range. The high-temperature Curie–Weiss fitting suggests that the antiferromagnetic coupling between RE 3+ and RE 3+ is dominant at low temperatures. The Arrott-plots imply that the magnetic transition in Tb 2 M TiO 6 is of second–order nature according to the Banerjee’s criteria. The magnetic entropy change − Δ S M is evaluated to be 10.7, 16.2 and 13.2 J kg −1 K −1 for Tb 2 CoTiO 6 , Tb 2 NiTiO 6 and Tb 2 CuTiO 6 at 4 K and magnetic field change Δ H = 6 T, respectively. The work suggests that the lack of 3 d –3 d coupling in the design of double perovskites is one of the potential approaches for developing low-temperature magnetic refrigeration materials.
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