BIORESOURCE TECHNOLOGY
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2023
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IF 11.4
Qiaozhi Zhang,Yuqing Sun,Weijian Xu,Yang Cao,Chunfei Wu,Chi-Hwa Wang,Daniel C.W. Tsang
Microwave (MW)-assisted catalytic degradation of organic pollutants draws increasing attention owing to its high efficiency in wastewater treatment. This work developed Cu-loaded biochar (CuBC) catalysts for time-efficient mineralization of refractory and high-concentration oxytetracycline (OTC). With only 1 min at 80 °C, Na 2 S 2 O 8 achieved 100% total organic carbon (TOC) removal over the Cu5BC, while NaClO mineralized 73.3% TOC over the metal-free BC, in contrast to a relatively low mineralization efficiency (< 35%) achieved by H 2 O 2 . The high efficiency in MW-assisted oxidation systems could be ascribed to reactive oxidizing species ( • SO 4 − or • ClO), which otherwise were barely detectable in a conventional heating system. The interactions between CuBC and MW were revealed by correlating the physiochemical characteristics to the MW absorption ability. The proposed catalytic systems can contribute to the development of a high-throughput and low-carbon wastewater treatment technology.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2022
·
IF 6.76
Yachun Ren,Yueyang Xu,Erjian Huang,Peng Zhang,Yongping Zeng
Adsorption desulfurization is a very effective method to remove thiophenic compounds from fuels. The metal–organic frameworks (MOFs) have emerged as a new type of desulfurization adsorbents because of their porous nature and large specific surface area. In this study, Cu 2+ was covalently introduced into the UiO-66 framework at the defective sites by the solvothermal method. Further, the π-complexation adsorbent UiO-66-Cu(I) containing Cu + for adsorption desulfurization was synthesized by the methanol vapor-induced reduction. The adsorption performance was tested for the removal of thiophene from the model fuels with different sulfur concentrations. In comparison with the pristine UiO-66, the adsorbent UiO-66-Cu(I) has a higher adsorption capacity for thiophene, reaching 14.8 mg S/g. The competitive adsorption results indicated that UiO-66-Cu(I) has good selectivity for thiophene in the presence of aromatic compounds. From the recycling experiments, this adsorption still has the 86 % of the initial capacity after four cycles, indicating that the adsorbent has a good recycling performance.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Shubin Cheng,Qian Lei,Coner Deng,Weixin Lei,Honglin Chen
A green protocol for refining industrial chemicals containing formaldehyde (FA) impurities is presented here for the first time. FA, as an unreactant or a byproduct, causes separation problems in many industrial processes. It can be removed to a level of less than 1 ppm with easily separable methanol formation using commercial Cu/ZnO/Al 2 O 3 catalyst at atmospheric pressure in the absence of external hydrogen. The formation of methanol is achieved by the transfer of hydrogen species generated with the assistance of water to free FA, affording high methanol selectivity (62 %). By investigating potential intermediates and implementing deuterium labeling experiments, together with carbon and hydrogen balance calculations, a plausible pathway of water-assisted FA removal is proposed. Moreover, the in situ generated hydrogen species can be transferred directly into unsaturated compounds for selective reduction.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Donglin Yang,Bingxiao Feng,Yaping Liu,Chaoting Deng,Hengjun Gai,Meng Xiao,Tingting Huang,Quanhong Zhu,Hongbing Song
The manner of ammonia-containing wastewater in industrial production has always been an urgent issue that needs to be solved. Accordingly, a carbon-supported low-loading Ru/Cu bimetallic catalyst with high activity and hydrothermal stability was produced through facile disposal for catalytic wet air oxidation (CWAO). In the preparation process, Ru and Cu ions were loaded onto micro mesoporous carbon prepared through the calcination of potassium citrate by impregnation. Various characteristic techniques were utilized to characterize their structures and morphology, and results show that the calcination temperature with micro-mesopores’ characteristics could regulate the morphology of carbon. The results of catalytic experiments demonstrated that the obtained catalyst showed excellent catalytic performance in the process of CWAO. The Ru/Cu@C-700 catalyst achieved 99.6 % conversion of ammonia water at 800 ppm and 99.1 % selectivity to nitrogen at 200 °C and 2 MPa O 2 in 4 h. The ammonia nitrogen content in the treated water was less than 15 ppm, meeting the standard for direct discharge . Moreover, no apparent deactivation phenomenon was observed after five cycles, indicating that the prepared catalyst can effectively prevent the leaching of ruthenium and copper nanoparticles . The low loading (less than 1 %) of the Ru/Cu bimetallic catalyst can significantly reduce costs and can synergistically enhance conversion and selectivity, providing an effective strategy for studying the CWAO of ammonia.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Xiaojing Cui,Yequn Liu,Wenjun Yan,Yanfeng Xue,Yangang Mei,Jiamei Li,Xiaoqing Gao,He Zhang,Shanhui Zhu,Yulan Niu,Tiansheng Deng
Suppressing reverse water-gas-shift (RWGS) reaction is high desirable but challenging and underdeveloped for Cu/ZnO catalysts, particularly for commercial Cu/ZnO/Al 2 O 3 catalysts. Different from the current methodologies to reduce RWGS reaction, we report a simply surface silylation method for efficiently minimizing RWGS reaction over a commercial Cu/ZnO/Al 2 O 3 catalyst. This method suppresses STY CO (Space-time yield) from 97.4 to 0.7 g CO ·kg cat −1 ·h −1 , improving STY MeOH from 20.2 to 39.9 g MeOH ·kg cat −1 ·h −1 and methanol selectivity from 15.1 to 92.9 mol%. The combination of characterization methods and density functional theory calculations provide insight into the suppressing mechanism of surface silylation on catalyst. A hydroxyl (on ZnO)-promoted RWGS reaction cycle is discovered, which can be efficiently inhibited by the consuming of hydroxyls via surface silyation. Our results provide a way to regulate RWGS reaction on Cu/ZnO-based catalysts and are expected to the further use of silylation strategy to tune the interconversion of CO and CO 2 via RWGS/WGS reaction on hydrogenation catalysts.
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Micromachines
·
2023
·Vol. 14
·期 7
·1318
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IF 3.4
Gang Li,Xuecheng Yu,Ruoyu Zhang,Qionglin Ouyang,Rong Sun,Liqiang Cao,Pengli Zhu
Copper-based nanoinks are emerging as promising low-cost alternatives to widely used silver nanoinks in electronic printing. However, the spontaneous oxidation of copper under ambient conditions poses significant challenges to its broader application. To address this issue, this paper presents an economical, large-scale, and environmentally friendly method for fabricating Cu@Ag nanoparticles (Cu@Ag NPs). The as-prepared nanoparticles exhibit a narrow size distribution of approximately 100 nm and can withstand ambient exposure for at least 60 days without significant oxidation. The Cu@Ag-based ink, with a 60 wt% loading, was screen-printed onto a flexible polyimide substrate and subsequently heat-treated at 290 °C for 15 minutes under a nitrogen atmosphere. The sintered pattern displayed a low electrical resistivity of 25.5 μΩ·cm (approximately 15 times the resistivity of bulk copper) along with excellent reliability and mechanical fatigue strength. The innovative Cu@Ag NPs fabrication method holds considerable potential for advancing large-scale applications of copper-based inks in flexible electronics.Keywords:core–shell nanoparticles;antioxidation;conductive ink;printing electronics
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ACS Applied Nano Materials
·
2023
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IF 5.9
Jingwen Feng,Jinjuan Gao,Wen Yang,Yaru Li,Jian Shi,Cong Liu,Mingshun Jiang,Shouzhen Jiang
Two-dimensional (2D) metal–organic frameworks (MOFs) have promising applications in surface plasmon resonance (SPR) sensing for their intriguing exciton migration and visible light-near infrared absorption properties. In this study, an effective biosensing structure comprising 2D Cu-TCPP MOF nanosheet-capsulated Au film was developed, such that lower molecular-weight dopamine with small changes of refractive index can be identified on the fiber-optic platform. The large areas of ultrathin 2D Cu-TCPP MOF nanosheets were well prepared, the experimental results indicated that the sensitivity (48%) and figure of merit (18%) were increased notably compared with the bare Au film. Moreover, the finite element method was adopted to numerically analyze and verify the excellent charge-transfer ability of MOF nanosheets and the bidirectional gain properties between MOF nanosheets and Au films. Furthermore, the sensitivity [1.24 nm/log(M)] and selectivity of the dopamine were significantly enhanced with a low limit of detection of 1.50 × 10–13 M and linear response with a wide range of concentrations from 5 × 10–12 M to 5 × 10–7 M through ssDNA surface modification and conformation amplification. As revealed by the above-mentioned results, the Cu-TCPP/Au/SMF biosensor can serve as a promising nanoplatform for clinical diagnosis and medical assessment.
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Small
·
2023
·Vol. 19
·期 45
·2302022
·
IF 13.3
Hai-Bing Zhao,Jia-Nan Huang,Qi Qin,Hong-Yan Chen,Dai-Bin Kuang
Rational design and facile synthesis of efficient environmentally friendly all-inorganic lead-free halide perovskite catalysts are of great significance in photocatalytic CO 2 reduction. Aiming at photogenerated charge carrier separation and CO 2 reaction dynamics, in this paper, a CsCuCl 3 /Cu nanocrystals (NCs) heterojunction catalyst is designed and synthesized via a simple acid-etching solution process by using Cu 2 O as the sacrificed template. Due to the disproportionation reaction of Cu 2 O induced by concentrated hydrochloric acid, Cu NCs can be deposited onto the surface of CsCuCl 3 microcrystals directly and tightly. As revealed by photoelectrochemical analysis, in situ Fourier transform infrared spectra, etc., the Cu NCs contribute a lot to extracting photoelectrons of CsCuCl 3 to improve the charge separation efficiency, regulating the CO 2 adsorption and activation, and also stabilizing the reaction intermediates. Therefore, CsCuCl 3 /Cu heterojunction exhibits a total electron consumption rate of 58.77 µmol g −1 h −1 , which is 2.9-fold of that of single CsCuCl 3 . Moreover, high CH 4 selectivity of up to 92.7% is achieved, which is much higher than that of CsCuCl 3 (50.4%) and most lead-free halide perovskite-based catalysts. This work provides an ingenious but simple strategy to rationally design cocatalysts in situ decorated perovskite catalysts for manipulating both the catalytic activity and the product selectivity.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yang Peng,Zhanwei Xu,Le Yu,Xucheng Li,Weiran Yang
The direct conversion of furfural (FUR) to 2-methyltetrahydrofuran (2-MTHF) was investigated over a trimetallic CuNiRe/Hβ catalyst. Under optimal reaction conditions at 240 °C under 3 MPa H 2 for 1 h, almost complete conversion of FUR and high-yield of 2-MTHF (81 %) was achieved. This is the highest yield reported for the direct conversion of FUR to 2-MTHF. HR-TEM demonstrated that the growth of Cu nanoparticles (NPs) on the surface of Hβ was inhibited after loading Ni or Re resulted in the smaller Cu particle size and better hydrogenation and hydrodeoxygenation activity. H 2 -TPR characterization exhibited that the reducibility of bimetallic and trimetallic catalysts was higher than that of monometallic catalysts·NH 3 -TPD explained that Hβ acid sites mainly contributed to FUR deoxygenation. The adsorption configurations of FUR, furfuryl alcohol (FOL) and 2-methylfuran (2-MF) on the catalyst were revealed by ATR-IR. Catalyst evaluation and control experiments proved that FUR was first hydrogenated to FOL, followed by hydrodeoxygenation to 2-MF, and finally hydrogenated to 2-MTHF catalyzed by the combination of three metals.
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MATERIALS CHEMISTRY AND PHYSICS
·
2022
·
IF 4.778
Xijun Li,Sifan Zhang,Lihua Zhu,Jun Liu,Huan Zhang,Ning Zhao,Bing Hui Chen
Herein, a series of the Pt-based bimetallic catalysts (PtM x /SBA-15) are gained by using ultrasonic incipient wetness impregnation method (M = Co, Cu, Ni or Zn). The experimental results show that the catalytic performance (including catalytic activity (turnover frequency-TOF), selectivity to crotyl alcohol) of PtCo x /SBA-15 for catalyzing crotonaldehyde selective hydrogenation is the best among PtM x /SBA-15. Additionally, the ratio of Pt/Co in the PtCo x /SBA-15 catalysts is changed to successfully synthesize PtCo/SBA-15, PtCo 2 /SBA-15, PtCo 5 /SBA-15. It demonstrates that the selectivity of the PtCo x /SBA-15 catalysts for crotonaldehyde selective hydrogenation to crotyl alcohol is significantly improved with the increase of the Co content. The PtCo 5 /SBA-15 catalyst provides 83.8% conversion of crotonaldehyde, 94.3% selectivity to crotyl alcohol and TOF of 910.5 h −1 under mild reaction conditions (3.0 MPa H 2 , 80 °C and 2.0 h). And PtCo 5 /SBA-15 has much better catalytic performance (higher catalytic activity and selectivity to crotyl alcohol) than PtCu 5 /SBA-15, PtNi 5 /SBA-15 and PtZn 5 /SBA-15. The reasons are as follows: (1) PtCo alloy forms, which is conducive to crotonaldehyde adsorption and activation; (2) there is an appropriate synergy effect between Pt and Co, greatly improving the capacity of the catalyst activating hydrogen under mild conditions; (3) the electron transfers from Co to Pt, resulting in the increase of Pt electron density and decrease of Co electron density, then the Co sites are advantageous to C O group adsorption and activation and Pt sites for H 2 adsorbing and activating; (4) with the increase of the Co proportion in PtCo x /SBA-15, the synergy effect between Pt and Co in PtCo alloy strengthens and thus increases the selectivity of C O group hydrogenation.
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ENERGY & FUELS
·
2022
·
IF 4.654
Ziyi Liu,Mengxue Wu,Jinfu Ma
Ammonia is a very promising source of carbon-free chemical energy. However, current electrochemical technologies for ammonia use are limited by the kinetically sluggish and easily toxic catalyst surface ammonia oxidation reaction (AOR). Here, we report an AOR catalyst in which Ni, Cu, and Co are highly dispersed on single-walled carbon nanotubes (CNTs) (Ni–Cu–Co/CNT) in the form of hydroxides and hydroxyl oxides by using a one-step solvothermal method. Ni–Cu–Co/CNT, with Co doping and a support of the CNT, has shown highly efficient catalytic activity for the AOR in alkaline media. Cyclic voltammetry tests show that the catalyst has an onset potential of 0.3 V vs Ag/AgCl and a peak current of 96 mA cm–2. Density functional theory suggests that the addition of Co and a CNT leads to a lower energy barrier for the critical AOR step, which can be attributed to intermetallic synergy and metal–support interactions formed by the CNT.
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Nano-Micro Letters
·
2022
·Vol. 14
·期 1
·1-13
·
IF 23.655
Li Xiaotong,Wang Jianghao,Lv Xiangzhou,Yang Yue,Xu Yifei,Liu Qian,Wu Hao Bin
Dual-site electrocatalysts with in situ formed metal-oxide interfaces are proposed and demonstrated to enhance the formation of multi-carbon products from electrochemical CO 2 reduction.
The 0.5-UiO/Cu delivers a high C2+ Faradaic efficiency of over 74% with notably boosted formation rate and durability, surpassing most reported electrocatalysts.
A unique mechanism of UiO-66 to induce in situ reconstruction of Cu surface and formation of UiO-66-derived amorphous ZrO x /Cu interface is uncovered, which improves the selectivity and productivity toward C2+ products.
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