CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Bolun Mei,Yueru Wang,Zhouxuan Zang,Ouyang Liu,Xu Liang,Guoji Liu,Han Sun,Xingchuan Yang,Li Xu
Calcination-driven Cu exsolution from a CuZr precursor tunes the Cu-ZrO 2 interfacial environment. • Catalysts with the optimal interfacial environment achieve ethanol selectivity approaching 90%. • Kinetic analysis and in situ DRIFTS support a dehydration‑hydrogenation pathway at the Cu-ZrO 2 interface. • DFT reveals that Cu-ZrO 2 interface converts high-barrier concerted dehydration into a lower-barrier stepwise route. The selective hydrogenolysis of ethylene glycol (EG) to ethanol is a critical step in the dimethyl oxalate (DMO)-to-ethanol process, yet the catalytically relevant Cu environment for this transformation remains insufficiently understood. Here, we prepared a series of CuZr catalysts with distinct Cu-ZrO 2 interfacial structures through calcination-induced structural evolution. Structural characterization reveals that calcination progressively redistributes Cu species from a more bulk-associated state in ZrO 2 to surface-enriched Cu, and ultimately to segregated Cu-rich domains. Among the catalyst series, calcination at an intermediate temperature of 550 °C gave the best performance. Ethanol yield scaled with the accessible Cu surface area, and both exhibited a volcano-type dependence on calcination temperature, whereas the Cu-normalized TOF decreased monotonically. This discrepancy underscores that exposed Cu alone cannot account for the catalytic behavior, and suggests an important contribution from coupled Cu-ZrO 2 interfacial environments. Kinetic analysis and in situ DRIFTS support a pathway involving dehydration-related transformation of EG followed by hydrogenation of carbonyl-type intermediates. DFT results further suggest that, relative to pristine ZrO 2 , the Cu-ZrO 2 interface stabilizes dehydration related carbon-containing intermediates, thereby enabling a more accessible stepwise pathway for EG dehydration and facilitating the subsequent hydrogenation to ethanol. These findings provide an interface engineering strategy for designing Cu-based catalysts in the DMO-to-ethanol process and related polyol hydrogenolysis reactions. Download: Download high-res image (129KB) Download: Download full-size image
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
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2022
·
IF 4.644
Yuewen Li,Yu Zhang,Xing Hou,Chunkun Lin,Degang Bu,Yalin Lan,Na Li,Shuyao Wu,Shuo Li,Xi-Ming Song
Seeking novel solar energy utilization and conversion methods has always been a frontier topic in energy research. Here, we propose a new way to directly photoelectrodeposit metals using solar energy based on semiconductor energy band theory . Three kinds of semiconductor photoanodes (TiO 2 , BiVO 4 and Fe 2 O 3 ) are employed to deposit metallic Cu or Bi at the cathode under illumination without external voltage. It is found that when TiO 2 and BiVO 4 are used as photoanodes, Cu, Cu 2 O and Bi can be continuously deposited on the cathode, but when Fe 2 O 3 photoanode is irradiated, no material comes out. The results prove that the potential of electrons in the conduction band determines whether photoelectric deposition occurs or not. The related mechanism involves the oxygen reduction reaction (OER) of the valence band holes of the photoanode, the collection of conduction band electrons by back electrode, as well as the reduction of metal ions on the counter electrode. In addition, we also put forward the concept of using the deposited Cu or Bi as the metal electrode to form a new metal-air battery to release chemical energy of the deposited metal.
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COMPOSITES SCIENCE AND TECHNOLOGY
·
2023
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IF 9.1
Bowen Cui,Chengguo Wang,Yanxiang Wang,Chengjuan Wang,Haotian Jiang,Mengfan Li,Zhenhao Xu
Cu nanoparticles were loaded on the surface of continuous carbon fibre (CF) and catalysed the growth of carbon nanotubes (CNTs) by continuous catalytic chemical vapour deposition . The results of Cu and traditional catalysts were contrastively studied in terms of surface morphology , microstructure and mechanical properties . It is reflected that the CNTs grown from Cu catalysts are in suitable distribution, with unique bamboo‐like structure and higher graphitisation degree. The carbon nanotube–carbon fibre utilising Cu catalyst has 53.0% higher interfacial shear strength than the pristine fibre, and shows advantage in tensile strength over its counterparts of traditional catalysts. Above all, a “loading–catalysis–reinforcing” mechanism was established, which theoretically and systematically explains how the nature of different catalyst metals affects the various stages in the process of growing CNT on the surface of continuous CF. This research expands the catalyst options, and develops the catalysis mechanism that offers an important theoretical guidance for the process optimization.
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COLLOIDS AND SURFACES B-BIOINTERFACES
·
2023
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IF 5.8
Yong-Qiang Xu,Liu-Yuan Zang,Hai-Yu Gao,Jin Peng,Dong-Yun Zheng,Chao Liu,Xiao-Jun Liu,Dong-Bing Cheng,Chun-Nan Zhu
Gd 3+ -doped quantum dots (QDs) have been widely used as small-sized bifunctional contrast agents for fluorescence/magnetic resonance (FL/MR) dual-modality imaging. However, Gd 3+ doping will always compromise the FL of host QDs. Therefore, balancing the Gd 3+ doping and the optical properties of QDs is crucial for constructing high-performance bifunctional nanoprobes . Additionally, most paramagnetic QDs are synthesized in the organic phase and need to be transferred to the aqueous phase for bioimaging. Herein, ingeniously designed shell-doped Cu-In-S/ZnS:Gd 3+ QDs have been prepared in the aqueous phase. It has been demonstrated that isolating paramagnetic Gd 3+ from fluorescent Cu-In-S core via doping Gd 3+ into ZnS shell not only avoided the decrease of FL quantum yield (QY), but also ensured the water accessibility of paramagnetic Gd 3+ ions, by which the FL QY and r 1 relaxivity of Cu-In-S/ZnS:Gd 3+ QDs achieved as much as 15.6% and 15.33 mM -1 ·s -1 , respectively. These high-performance QDs with excellent stability, low biotoxicity, and good tumor permeability were successfully applied for in vivo tumor FL/MR dual-modality imaging, and have shown significant potential in the precision detection and diagnosis of diseases.
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Frontiers in Energy Research
·
2023
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IF 3.4
Huang Jiamin,Zhang Guanghui,Wang Mingrui,Zhu Jie,Ding Fanshu,Song Chunshan,Guo Xinwen
The catalytic production of higher alcohols (HAs) is a promising path for converting CO2 into value-added chemical products. The application is still limited by the low selectivity of HAs (less than 10%) on most catalysts. Here, we report a tandem catalyst consisting of Mn-Cu-K modified iron carbide and CuZnAlZr catalyst. The modification of iron carbide with Mn, Cu and K promoters improves the formation of HAs (13.5% Sel.), and the construction of tandem catalysts with CuZnAlZr can further enhance the catalytic performance. By examining different catalyst filling methods and the filling ratio of the tandem catalyst, it was found that the powder mixing resulted in a higher selectivity of HAs with a mass ratio of the two components of 1:1, and a synergistic effect leads to a higher selectivity of HAs (15.5%) with about 40% of propanol and butanol among HAs.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 11
·2211845
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IF 19
Chuan Fan,Yong Luo,Meng Tian,Mengyun Zhou,Lirong Wang,Tailin Xu,Xueji Zhang
“Green Synthesis” has been broadly applied in drug synthesis and nanomaterial preparation. The integration of automated micro-synthesis and high-throughput screening systems is a key way to achieve the goal of green manufacturing. Here, a one-click green synthesis platform is designed that integrates droplets arrays-based micro-synthesis for Raman enhancement performance high-throughput screening of MNPs@Cu-MOF (AuNPs@, AgNPs@, PtNPs@Cu-MOF) under room temperature and normal pressure. The fully integrated ultrasound units can achieve rapid multi-component mixing in the droplet array systems, and significantly accelerate materials growth as well as enhance encapsulation of noble metal nanoparticles into Cu-MOF structures. Based on such integrated systems, structures with high Raman enhancement performance can be high-throughput evaluation and easily screened out. The results indicated that the AgNPs@Cu-MOF exhibited the best Raman enhancement performance, which is ≈8 times higher than pure AgNPs. Such a green and integrated platform provides a way for automated multi-type composites fabrication, which can be expanded to multiple fields in the future via combined robotic platforms and artificial intelligence technology.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Guangyu Duan,Xintong Li,Xin Ma,Wei Zhong,Shuai Wang
Cu/Ni-bearing wastewater contamination has recently been a challenge for the environmental protection worldwide. Herein, a novel poly(2-acrylamide-pentanedihydroxamic acid) (PAPDA) resin containing –CONHOH and –COOH groups was prepared and applied to effectively remove Cu 2+ and Ni 2+ from heavy metal wastewater. The batch adsorption experiments revealed that the maximum adsorption capacities of PAPDA resin for Cu 2+ and Ni 2+ were 436.08 and 195.05 mg·g −1 , respectively, which were 10.20 and 9.45 times higher than that of polyacrylic resin . Specifically, the adsorption kinetics and thermodynamics of PAPDA were respectively consistent with the pseudo-second-order kinetic model and the Langmuir isotherm model, indicating that the adsorption is a single-layer chemisorption process. Besides, the adsorption mechanism was investigated by SEM, XRD, FT-IR, XPS, DFT calculations, suggesting that the PAPDA resin possessing abundant active sites could effectively adsorb the heavy metal ions . Noticeably, the –CONHOH groups represented the strong affinity towards Cu 2+ and Ni 2+ by forming stable five-membered rings. In addition, column experiments were conducted to study the practical adsorption process of PAPDA resin to heavy metal ions. Overall, the results proved that the novel PAPDA resin as a green and highly efficient adsorbent has a promising potential for the treatment of heavy metals-containing wastewater.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Luwei Wang,Chenliu Tang,Pengfei Huang,Xiang Hu,Zhirong Sun
The widespread detection and potential adverse effects of antibiotics in the aquatic environment call for effective treatment technology. Electro-Fenton is a promising strategy, but the preparation of efficient and stable cathodes is still challenging. In this study, a novel metal-organic framework (MOF)-derived N-doped cathode Fe/Cu-C400Ar was synthesized successfully for the degradation of ceftazidime (CAZ) in heterogeneous electro-Fenton (hetero-EF) system. The doping of copper could enhance electrocatalysis with a high electrochemical surface active area and low resistance. Fe/Cu-C400Ar cathode achieved CAZ removal efficiency of 99.5 ± 0.4% within 120 min, and it exhibited excellent stability after six recycle runs. Quenching experiments and electron paramagnetic resonance (EPR) tests proved that the primary species was hydroxyl radical during the CAZ degradation. In addition, the degradation pathway of CAZ was proposed including the cleavage of the pyridine ring and the shedding of the thiazole ring. Moreover, the prediction of intermediates toxicity by Ecological Structure Activity Relationships (ECOSAR) software indicated the environmentally friendly features of the CAZ degradation process. This study provided a promising cathode for the electrocatalytic degradation of antibiotic wastewater in hetero-EF system.
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APPLIED BIOCHEMISTRY AND BIOTECHNOLOGY
·
2022
·Vol. 195
·期 2
·1216-1230
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IF 3.094
Cheng Qiaojuan,Chi Xinyu,Liang Yingchao,Li Wanxin,Sun Jiaxin,Tao Jin,Wang Zhi
Metal–organic frameworks (MOFs) can be used as the immobilization carriers to protect the physicochemical properties of enzymes and improve their catalytic performance. Herein, we report an in situ co-precipitation method to immobilize lipase from Candida sp. 99–125 in Cu-BTC MOF (BTC = 1, 3, 5-benzene tricarboxylic acid, H 3 BTC). Characterizations of the immobilized lipase (lipase@Cu-BTC) have confirmed the entrapment of lipase molecules in Cu-BTC MOF. The immobilized lipase has been successfully applied for resolving N- hydroxymethyl vince lactam ( N -HMVL) and its catalytic activity is five times that of native enzyme. More importantly, we found that Cu-BTC MOF can afford powerful protection for enzyme in nearly dry organic solvent and endow the immobilized lipase with excellent reusability and storage stability. Our present study may widen the application of immobilized enzyme with MOF as the immobilized carrier. Graphical Abstract
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Catalysts
·
2022
·Vol. 12
·期 11
·1363
·
IF 4.501
Haimei Chen,Shaofei Wang,Lilan Huang,Leitao Zhang,Jin Han,Wanzheng Ren,Jian Pan,Jiao Li
The preparation of heterogeneous Fenton catalysts with both adsorption and catalytic properties has become an effective strategy for the treatment of refractory organic wastewater. In this work, 4A-Fe@Cu bimetallic Fenton catalysts with a three-dimensional core-shell structure were prepared by a simple, template-free, and surfactant-free methodology and used in the adsorption and degradation of Congo red (CR). The results showed that the open three-dimensional network structure and the positive charge of the surface of the 4A-Fe@Cu catalyst could endow a high adsorption capacity for CR, reaching 432.9 mg/g. The good adsorption property of 4A-Fe@Cu for CR not only did not inactivate the catalytic site on 4A-Fe@Cu but also could promote the contact between CR and the active sites on the catalyst surface and accelerate the degradation process. The 4A-Fe@Cu bimetallic catalyst exhibited higher catalytic activity than monometallic 4A@Cu and/or 4A-Fe catalysts due to low work function value. The effects of different pH, H2O2dosages, and catalyst dosages on the catalytic performance of 4A-Fe@Cu were explored. In the conditions of 7.2 mM H2O2, 2 g/L 4A-Fe@Cu, and 1 g/L CR solution, the degradation ratio of CR by 4A-Fe@Cu could reach 99.2% at pH 8. This strategy provided guidance to the design of high-performance Fenton-like catalysts with both adsorption and catalysis properties for dye wastewater treatment.Keywords:fenton reaction;Fe/Cu bimetallic catalyst;congo red;adsorption;catalysis
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2022
·Vol. 98
·期 2
·506-515
·
IF 3.709
Cao Shuang,Zhang Haixiang,Wang Xueman,Peng Miquan,Huang Renhua,Hong Wei,Fu Hailu,Chen Xiongbo,Lin Zejian
In SCR denitrification technology, the conventional coprecipitation method has the disadvantages of high temperature and difficulty in controlling the precipitation rate. Various Ce x CuTiO 2 catalysts were synthesized using ice-melting (Ce x CuTi-Ice) and conventional coprecipitation (Ce x CuTi-Con) methods for the selective catalytic reduction (SCR) of NO with NH 3 . Ce 0.4 CuTi-Ice catalyst exhibited excellent catalytic activity among the Ce x CuTiO 2 catalysts, and 80% NO x conversion was achieved within a temperature range of 250–375 °C, exceeding that of Ce 0.4 CuTi-Con catalyst by 20%; in addition, N 2 selectivity was nearly 100%. To elucidate the release characteristics of the precursor solution during ice-melting synthesis, the changes of Cu and Ce concentrations in the solution were investigated by ICP-OES. The precursor solution was released at a slow rate via the ice-melting method, resulting in a large surface area, small crystallite sizes, and effective uniform nanoparticles with abundant active species and increased surface acidity. The promoted mechanism could be attributed to the enhanced oxidation of NO to NO 2 at low temperatures and the rapid reaction between NO species and coordinated NH 3 at high temperatures. © 2022 Society of Chemical Industry (SCI).
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Journal of Cleaner Production
·
2023
·
IF 11.1
Yaoyao Zhang,Kangze Yuan,Luca Magagnin,Xishe Wu,Zhenyi Jiang,Wei Wang
Mercapto-functionalized aerogels (MA-X) were fabricated using γ-mercaptopropyltrimethoxysilane (MPTMS) as a modification reagent to eliminate Pb (II) and Cu (II) ions from wastewater. Mercapto-functionalized aerogel (MA2) with the MPTMS/TEOS molar ratio of 0.5 exhibited the maximum adsorption amounts of 163.99 mg/g for Pb (II) and 172.41 mg/g for Cu (II) in single ion system, respectively. In binary ion system, selective adsorption experiments revealed that the equilibrium adsorption capacity for Cu (II) (161.29 mg/g) was significantly greater than Pb (II) (90.42 mg/g), and the selectivity factor α showed greater selectivity for Cu (II), demonstrating that Cu (II) was more readily adsorbed on MA2. The results showed that adsorption was consistent with pseudo-second order model and Langmuir model. Thermodynamic results demonstrated that adsorption phenomenon was an exothermic reaction that occurred spontaneously. XPS analysis and density functional theory (DFT) simulations showed that the main mechanism for the adsorption of Pb (II) and Cu (II) on MA2 was through coordination chelation of the –SH groups with Pb (II) and Cu (II). DFT calculations showed a lower adsorption energy (E ads ) of Cu (II) (−2.72 eV) with respect to Pb (II) (−0.80 eV), indicating that Cu (II) was more stably adsorbed on MA2 and more difficult to exchange by Pb (II). In order to determine the environmental impact of the MA2 preparation process, a life cycle assessment (LCA) was conducted and contribution of each material to MA2 production was analyzed. Finally, a strategy that is environmentally friendly and effective has been proposed in order to facilitate MA-X adsorbents production and to improve their application for the treatment of heavy metal polluted wastewater.
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