ADVANCED MATERIALS
·
2023
·
IF 29.4
Yingzhen Wei,Shuang Wang,Mengyang Chen,Jinfeng Han,Guoju Yang,Qifei Wang,Jiancheng Di,Hongli Li,Wenzheng Wu,Jihong Yu
Core–shell catalysts with functional shells can increase the activity and stability of the catalysts in selective catalytic reduction of NO x with ammonia x . However, the conventional approaches based on multistep fabrication for core–shell structures encounter persistent restrictions regarding strict synthesis conditions and limited design flexibility. Herein, a facile coaxial 3D printing strategy is for the first time developed to construct zeolite-based core–shell monolithic catalysts with interconnected honeycomb structures, in which the hydrophilic noncompact silica serves as shell and Cu-SSZ-13 zeolite acts as core. Compared to a Cu-SSZ-13 monolith which suffers from the interfacial diffusion, the SiO 2 shell layer can increase the accessibility of active sites over Cu-SSZ-13@SiO 2 , resulting in a 10–20% higher NO conversion at200−550 °C under 300 000 cm 3 g −1 h −1 . Meanwhile, a thicker SiO 2 shell enhances the hydrothermal stability of the aged catalyst by inhibiting the dealumination and the formation of CuO x . Other representative monolithic catalysts with different topological zeolites as shell and diverse metal oxides as the core can be also realized by this coaxial 3D printing. This strategy allows multiple porous materials to be directly integrated, which allows for flexible design and fabrication of various core–shell monolithic catalysts with customized functionalities.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 29
·13638-13645
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IF 3.3
Yuan Gao,Bo Liu,Hanlu Xu,Caixia Shi,Ning Yan,Shaorong Wang,Rongli Jiang
To meet the growing demand for clean and sustainable energy, the development of high-performance proton conductive materials is crucial for practical applications in PEMFCs. However, the current materials suffer from issues such as low conductivity, poor durability, and unclear structure–activity relationship. To address these challenges, we investigate the proton conductivity properties of lysine-decorated Cu-BTC (where BTC is benzene-1,3,5-tricarboxylate) and its corresponding thin-film membrane. We explore the impact of lysine (Lys) content (10 wt%, 20 wt%, 30 wt%, and 40 wt%) on the proton conductivity performance under varying humidity and temperature conditions. Our findings show that Cu-BTC-Lys (40 wt%) exhibits the best conductivity of 1.2 × 10−3 S cm−1 at 80 °C under 100% relative humidity (RH), aided by an activation energy (Ea) of 0.25 eV facilitating proton transfer through hydrogen-bonding networks via the Grotthuss mechanism. We then create a proton conductive membrane by fabricating Cu-BTC-Lys (40 wt%) with the PVP/PVDF polymeric matrix. The resulting Cu-BTC-Lys@PVP/PVDF-20 membrane shows a significantly improved conductivity of 4.8 × 10−3 S cm−1 at 80 °C under 100% RH, along with a decreasing Ea value of 0.15 eV. The membrane retains its rich hydrogen-bonding networks and excellent performance durability for up to 5 days, making it an ideal candidate for real-life applications.
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Jianping Ai,Yaping Shuai,Min Hu,Lihong Cheng,Siling Luo,Wenkui Li,Zhiqin Chen,Liling Hu,Zehua Zhou
A novel class of high-entropy (HE) spinel ferrites (Mg 0.2 Co 0.2 Ni 0.2 Cu 0.2 Zn 0.2 )Fe 2 O 4 , have been successfully synthesized by the solution combustion synthesis method followed by heat-treatment at 500–1500 °C. The resultant spinel ferrites were systematically investigated by various methods including XRD , SEM, TEM, EDS, Raman spectra, etc. It was demonstrated that the entropy drives a reversible transformation between a single-phase state and multiphase. And the entropy predominates the thermodynamic landscape. The as-fabricated high-entropy (Mg 0.2 Co 0.2 Ni 0.2 Cu 0.2 Zn 0.2 )Fe 2 O 4 solid solution is single-phase with homogeneous transition-metal element distribution. Moreover, a trade-off between grain growth and crystallization during heat-treatment process; the average grain size of product is only 352.96 nm after being annealed at 1000 °C for 3 h probably due to “sluggish diffusion effect”. The resultant HE spinel ferrites (Mg 0.2 Co 0.2 Ni 0.2 Cu 0.2 Zn 0.2 )Fe 2 O 4 were first used as a heterogeneous catalyst of peroxodisulfate (PDS). Compared with basic solution condition, the HE spinel ferrite/PDS system exhibited a higher degradation rate for the removal of rhodamine B (RhB) and tetracycline (TC) at initial pH range of 3.0–5.1. Both the hydroxyl radicals and sulfate radicals played an important role on RhB and TC degradation. The high catalytic efficiency and good stability of high-entropy (Mg 0.2 Co 0.2 Ni 0.2 Cu 0.2 Zn 0.2 )Fe 2 O 4 catalyst demonstrates that it is suitable for application in wastewater disposal.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Yongpan Shan,Yajie Ma,Changcai Wu,Xiangliang Ren,Xianpeng Song,Dan Wang,Hongyan Hu,Xiaoyan Ma,Yan Ma
Control release of pesticides based on target plant characteristics is highly desirable for improving the effective utilization rate and reducing non-target organism risks. Here, the controlled release formulations (Cu-CS@IN@MIL-100 (Fe)) were successfully prepared by employing MIL-100 (Fe) as the carrier material, indoxacarb (IN) as the model pesticide, and chitosan (CS) as a coating to chelate copper ions by chemical crosslinking. The prepared Cu-CS@IN@MIL-100 (Fe) had an acceptable loading content (36.25 %). The introduction of CS and copper ions endowed it with sustained release properties under weak acidity conditions like cotton leaves. The laboratory bioassay experiments showed that Cu-CS@IN@MIL-100 (Fe) had practical good insecticidal activity (LC 50 = 4.936 mg/L) in controlling Helicoverpa armigera larvae. For long-term control efficacy experiments, after 14 days of application, the Cu-CS@IN@MIL-100 (Fe) treatment (73 %) mortality of Helicoverpa armigera larvae was significantly higher than the 15 % indoxacarb suspension concentrates (SC) treatment (27 %). Moreover, Cu-CS@IN@MIL-100 (Fe) had no adverse effect on cottonseed germination and the acute toxicity to Chrysopa pallens larvae was significantly lower than IN SC. Therefore, MIL-100 (Fe) could be used as an ecological safety carrier for pesticide delivery to improve IN effective utilization and reduce non-target organism risks.
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MOLECULES
·
2023
·Vol. 28
·期 6
·2687
·
IF 4.6
Liudi Ji,Qi Wang,Xiaqing Gong,Jiamin Chen,Xiaoming Zhu,Zeyu Li,Peng Hu
Dopamine (DA) is an important neurotransmitter. Abnormal concentration of DA can result in many neurological diseases. Developing reliable determination methods for DA is of great significance for the diagnosis and monitoring of neurological diseases. Here, a novel and simple electrochemical sensing platform for quantitative analysis of DA was constructed based on the Cu-TCPP/graphene composite (TCPP: Tetrakis(4-carboxyphenyl)porphyrin). Cu-TCPP frameworks were selected in consideration of their good electrochemical sensing potential. The graphene nanosheets with excellent conductivity were then added to further improve the sensing efficiency and stability of Cu-TCPP frameworks. The electrochemical properties of the Cu-TCPP/graphene composite were characterized, showing its large electrode active area, fast electron transfer, and good sensing performance toward DA. The signal enhancement mechanism of DA was explored. Strong accumulation ability and high electrocatalytic rate were observed on the surface of Cu-TCPP/graphene-modified glassy carbon electrode (Cu-TCPP/graphene/GCE). Based on the synergistic sensitization effect, an ultrasensitive and simple DA electrochemical sensor was developed. The linear range is 0.02–100 and 100–1000 µM, and the detection limit is 3.6 nM for the first linear range. It was also successfully used in detecting DA in serum samples, and a satisfactory recovery was obtained.
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高影响因子
MOLECULES
·
2023
·Vol. 28
·期 8
·3511
·
IF 4.6
Xingfan Gong,Jiacheng Xu,Tiantian Zhang,Yan Sun,Shiyu Fang,Ning Li,Jiali Zhu,Zuliang Wu,Jing Li,Erhao Gao,Wei Wang,Shuiliang Yao
Cu-doped manganese oxide (Cu–Mn2O4) prepared using aerosol decomposition was used as a CO oxidation catalyst. Cu was successfully doped into Mn2O4due to their nitrate precursors having closed thermal decomposition properties, which ensured the atomic ratio of Cu/(Cu + Mn) in Cu–Mn2O4close to that in their nitrate precursors. The 0.5Cu–Mn2O4catalyst of 0.48 Cu/(Cu + Mn) atomic ratio had the best CO oxidation performance, withT50andT90as low as 48 and 69 °C, respectively. The 0.5Cu–Mn2O4catalyst also had (1) a hollow sphere morphology, where the sphere wall was composed of a large number of nanospheres (about 10 nm), (2) the largest specific surface area and defects on the interfacing of the nanospheres, and (3) the highest Mn3+, Cu+, and Oads ratios, which facilitated oxygen vacancy formation, CO adsorption, and CO oxidation, respectively, yielding a synergetic effect on CO oxidation. DRIFTS-MS analysis results showed that terminal-type oxygen (M=O) and bridge-type oxygen (M-O-M) on 0.5Cu–Mn2O4were reactive at a low temperature, resulting in-good low-temperature CO oxidation performance. Water could adsorb on 0.5Cu–Mn2O4and inhibited M=O and M-O-M reaction with CO. Water could not inhibit O2decomposition to M=O and M-O-M. The 0.5Cu–Mn2O4catalyst had excellent water resistance at 150 °C, at which the influence of water (up to 5%) on CO oxidation could be completely eliminated.Keywords:doping;Cu–Mn2O4;CO oxidation;oxygen vacancy;water resistance;DRIFTS-MS
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CHEMICAL PHYSICS LETTERS
·
2023
·
IF 2.8
Lei Xia,Yi Lu,Yuan-Zhou Li,Zhi-Yi Hu,Xiao-Yu Yang
Photocatalytic hydrogen production from seawater has great prospects for generating clean energy from renewable resources. We designed a TiO 2 -rGO-Cu photocatalyst that possesses a pathway for directed electron transfer from nitrogen-doped TiO 2 to rGO and then to Cu nanoparticles, which leads to efficient electron-hole pairs separation. Results show that TiO 2 -rGO-Cu has a hydrogen production rate of 16.08 mmol h −1 g −1 in simulated seawater, which is as much as 25 times higher than that of TiO 2 . The mechanism for a highly efficient directional interfacial electron transport is proposed. The strategy could be effective for designing new photocatalysts for hydrogen production from seawater.
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Catalysts
·
2023
·Vol. 13
·期 4
·673
·
IF 3.9
Jinghu Zhu,Hui Liu,Xueyan Zhou,Zhijun Wang,Liancheng Bing,Dezhi Han,Guangjian Wang,Fang Wang
Cu-based catalysts, modified by gallium addition via the stepwise co-precipitation method, were studied for the liquid phase hydrogenation of hydroxypivalaldehyde (HPA) to neopentyl glycol (NPG). Through physico-chemical techniques, the effects of gallium introduction on the Cu trimetallic catalyst performance and the reaction mechanism of HPA hydrogenation were discussed. The characterization results showed that gallium introduction can influence the dispersion, reduction, and distribution of active Cu species, as well as their reactivity. Herein, the catalyst with 2 wt% gallium addition exhibited excellent catalytic performance with HPA conversion rate and NPG selectivity of 93.5% and 95.5%, at a reaction pressure of 3 MPa, temperature of 110 °C, hydrogen-aldehyde ratio (molar ratio) 10:1, and liquid space-time at a speed of 8.4 h−1. The good performance could be attributed to gallium doping tending to dynamically tune the interaction between the components, increasing Cu dispersion and the distributions of Cu+and Cu0species on the catalyst surfaces.Keywords:HPA hydrogenation;NPG synthesis;Cu-based catalyst;gallium modification;Cu+/Cu0
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COLLOIDS AND SURFACES B-BIOINTERFACES
·
2023
·
IF 5.8
Chan Li,Sheng Zhou,Chuncheng Chen,Lijun Zhu,Shijie Li,Zhuoyue Song,Jian Liang,Chunzhi Tang,Nenggui Xu,Tao Liu,Shihui Liu
Disulfiram (DSF), a drug for alcohol withdrawal , has attracted extensive scientific attention due to its potential to treat cancer. The metabolite of DSF, diethyl dithiocarbamate (DDTC), forms a Cu-DDTC complex in vivo with copper ions , which has been shown to be a proteasome inhibitor with high antitumor activity . However, the in vivo stability of Cu-DDTC complexes remains a challenge. In this study, the nanomedicine [email protected] with high antitumor activity was prepared by using the nanoscale metal-organic framework (MOF) Cu-BTC as a carrier and loading diethyldithiocarbamate (DDTC) through coordination interaction. The results showed that [email protected] had high drug loading and adequate stability, and exhibited DDTC-Cu(I) chemical valence characteristics and polycrystalline structure features. In vitro cytocompatibility investigation and animal xenograft tumor model evaluation demonstrated the anti-cancer potential of [email protected] , especially the combination of [email protected] with low-dose cisplatin showed significant antitumor effect and biosafety. This study provides a feasible protocol for developing antitumor drugs based on the drug repurposing strategy.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Xiaoqi Liu,Yanyun Zhang,Yan Liu,Ting'an Zhang
Chitosan bead grafted by third-generation dendrimers (CB-G3) with a diameter of 1.40 mm was synthesized to investigate their performance in recovering Ag(I), Cu(II), and Pb(II) ions in aqueous media. The prepared adsorbents were characterized by XRD, FT-IR, elemental analysis, TGA , and SEM, and the effects of pH, contact time, concentration, and temperature were examined. The results showed that the adsorbents were successfully fabricated. The optimum pH value was 5, and the increased generation number contributed to adsorption capacity improvement, indicating that electrostatic interactions between amine groups and metal ions are the governing mechanism of adsorption by the CB-G3. The kinetics, isotherms, and thermodynamics of Ag(I), Cu(II), and Pb(II) adsorption onto the CB-G3 were investigated. The adsorption processes can be described using pseudo-second-order kinetic and Langmuir models. The maximum monolayer adsorption capacities were 105.62, 88.82, and 97.87 mg·g −1 for Ag(I), Cu(II), and Pb(II) at 30 °C within 210 min, respectively. Electrostatic interactions and hydrogen bonds are the main mechanisms between metal ions and N atoms. Therefore, the CB-G3 is a promising candidate for Ag(I), Cu(II), and Pb(II) adsorption owing to its splendid ability in easy separation, good adsorptivity, and reusability for efficiently adsorbing Ag(I), Cu(II), and Pb(II) ions.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Rui Zhang,Feifei Chen,Haokun Jin,Yong Zhang,Xiaoya Hao,Yingda Liu,Tianming Feng,Xinghua Zhang,Zunming Lu,Weihua Wang,Feng Lu,Hong Dong,Hui Liu,Hui Liu,Yahui Cheng
In Cu-based electrocatalysts, appropriate amount of Cu 0 and high concentration of Cu + are essential for the efficient conversion of CO 2 into C 2+ products. An obstacle of CO 2 electroreduction is the inevitable reduction of Cu + to Cu 0 at cathodic potential. Intermediates confinement is a promising solution to delay Cu + deterioration, in which it is crucial to maintain an appropriate amount of Cu 0 and Cu + species to produce sufficient intermediates to protect most Cu + species. Herein, based on the influence of Cu + /Cu 0 ratio on the reaction process and its feedback, a series of hollow Cu 2 O nanoreactors with different cavity sizes were synthesized to modulate the concentration of intermediates and the coverage degree of Cu + , so as to realize a constant high Cu + /Cu 0 ratio. The optimized hollow Cu 2 O nanoreactors achieved a C 2+ Faradaic efficiency of 70.1 ± 0.2 % at a partial current density of −9.3 ± 0.1 mA cm −2 over 30 h and a large C 2+ -to-C 1 ratio of 9.73. Operando Raman spectra and quasi in - situ Auger electron spectra confirmed that the moderate cavity Cu 2 O nanoreactors led to a full coverage of Cu + and an optimal Cu + /Cu 0 ratio of 8.12:1, which brought the stability of Cu + species and cavity structure, as well as the enhanced C C dimerization.
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JOURNAL OF LUMINESCENCE
·
2022
·
IF 4.171
Lijin Wang,Zhongyuan Guan,Zhenyang Liu,Ouyang Lin,Wenrong Cui,Zhe Yin,Aiwei Tang
The interplay between ZnS shelling reaction and cation exchange affected the genuine nanostructure of the multinary Cu–In–S-based nanocrystals (NCs), which arose from the dosage and injection speed of Zn precursors as well as the surface of the seed NCs. The effects of Zn precursors on the growth of Cu–In–Zn–S NCs have been previously reported. However, effective control of cation exchange based on the surface of seed NCs is still lacking. Herein, a seed-mediated growth method was developed to eliminate the instability of free ligands and ions on the seed NCs. The clean surface of seed NCs was critical for balancing the internal cation exchange and epitaxial shelling reaction of NCs. Importantly, the photoluminescence quantum yield of the Cu–In–Zn–S NCs has been improved without peak shift through this method. In this dynamic balanced process, the as-obtained Cu–In–Zn–S NCs were confirmed to be gradient alloyed structures rather than core-shell structures. Furthermore, this method can be used to synthesize green- and red-emission Cu-In-Zn-S NCs as well. This seed-mediated strategy through simple redispersion may pave a way toward the controllable synthesis of NCs with gradient alloyed structures.
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