RESEARCH ON CHEMICAL INTERMEDIATES
·
2026
·
IF 3.3
Xu Ying-Yu,Wang Shuang,Zhu Han-Dong,Wang Shuo,Feng Xiao-Qian,Wang Huan,Zhao Yong-Hua
Photo-thermal synergistic catalysis offers a promising route for low-temperature and efficient hydrogen production, in which the design of catalysts is crucial. In this study, a series of promoter-modified Cu supported on ZnO (M-Cu/ZnO, M = Al, Zr, Co, Ce) were designed and prepared via a controllable hydrothermal synthesis strategy, and their catalytic performance in photo-thermal methanol steam reforming (MSR) for hydrogen production was systematically investigated. By varying the type of promoter, precise modulation of the catalyst's textural properties, metal-support interactions, and distribution of active sites was achieved. Characterization results revealed that the introduction of Al promoters significantly enhanced the dispersion of Cu species on the ZnO surface and strengthened metal-support interactions, thereby effectively suppressing the sintering and deactivation of active components during the reaction. Under photo-thermal MSR conditions of 240 °C, 0.1 MPa, and a space velocity of 17 300 mL·g −1 ·h −1 , the Al-Cu/ZnO catalyst exhibited the optimal catalytic performance, achieving a methanol conversion of 97.08% and an H 2 yield of 99.14 mL·g −1 ·min −1 , with only an 11% decrease in conversion after 10 h of continuous operation, demonstrating excellent stability. This work elucidates the structure–activity relationships in multicomponent Cu/ZnO catalysts for photo-thermal MSR from the perspective of promoter engineering, providing both experimental evidence and design insights for the development of efficient and stable solar-driven hydrogen production catalyst systems.
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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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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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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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高影响因子
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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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Fei Zhong,Chunlin Chen,Daiyu Zhang,Rui Yang,Xusong Huang,Kai Yang,Haoqing Qin,Xulin Yang
Polyaniline (PANI), a polymer with a high nitrogen content, has been shown to have good flame retardant properties. Here, we significantly improved the self-carbon formation ability of PANI at high temperature by doping with phytic acid (PA). Meanwhile, a new organic-metal ion flame retardant (DPANI/PA@Cu) was obtained by introducing Cu 2+ with catalytic carbon formation property into PANI/PA using the complexation between transition metal ions and PA. Surprisingly, the introduction of metal ions was also able to trigger the formation of dendritic structure of PANI (DPANI), which is important for its dispersion in resin matrix and strengthening effect on the coating. The test results demonstrated that the composite coating with 5% content of DPANI/PA@Cu had the lowest back-side temperature (174.9 ℃), the highest expansion height (18.5 mm) and the lowest smoke density class (45.3%). In addition, the DPANI/PA@Cu 5% /EP composite coating retained the maximum amount of residual carbon (29.7%), which was mainly related to the synergistic catalytic effect of PA and Cu 2+ . Ultimately, the retained PANI residual carbon and CuO nanoparticles diffused in the char layer acted as interceptors for the external flame and heat.
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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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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Xiuting Wu,Zefeng Zheng,Liang Ma,Changsong Hu,Yunhong Pi,Tiejun Wang
The aqueous-phase reforming of methanol(APRM)via non-precious metal heterogeneous catalysts is highly desirable, but challenging. Herein, we report a highly efficient copper catalyst encapsulated by chitosan-glucose (CS-G) conjugate with high metal loading of 35 wt% for H 2 generation from APRM. The optimized Cu@CS 19 -G 1 -300 catalyst exhibited exceptional activity of 1.39 × 10 5 μmol H2 /g cat /h at low temperature of 210 °C, which was ∼4.5 times higher than that of commercial CuZrAl catalysts (2.88 × 10 4 μmol H2 g cat −1 h −1 ). The chitosan-glucose conjugate acted not only as the main carbon support for Cu dispersion, but also as adsorbent to stablize as many Cu ions as possible. And meanwhile, with abundant Cu + /Cu 0 interface sites due to the reducing effect of glucose, the water gas shift reaction (WGSR) was intensified and thus displayed excellent selectivity toward CO by-product. This specific catalyst construction for H 2 production from APRM exhibits great potential of on-site H 2 supply for polymer membrane fuel cells.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jingyun Zhang,Zhen Jia,Shitao Yu,Shiwei Liu,Lu Li,Congxia Xie,Qiong Wu,Youzheng Zhang,Hailong Yu,Yuxiang Liu,Jinhui Pang,Yue Liu
Controllable carbonyl group (C O) hydrogenation is the key to the transformation of furfural molecules into high-value furfuryl alcohol chemicals. Herein, a non-noble copper metal catalyst (Cu/MgO) was prepared for the efficient hydrogenation of furfural to furfuryl alcohol under mild conditions. At 383 K and 2 MPa H 2 , 99.9% conversion of furfural with 99.9% selectivity to furfuryl alcohol was achieved within 80 min while the turnover frequency (TOF) was 56.87 h −1 . The temperature of a reductive pretreatment can be used to tune the nature of the interfaces between reduced copper and the metal oxides present in copper-magnesium oxide catalysts. The valence copper species exhibited unique catalytic properties in the hydrogenation of furfural to furfuryl alcohol. Besides, the Cu/MgO-350 exhibited excellent stability and reusability without significant activity loss. These results were accounted for by the MgO alkaline interface contributing to the effective formation and high dispersion of different valence Cu species. The active site had strong adaptability to the adsorption of reactants and desorption of products, thus avoiding excessive hydrogenation of furfural. According to the analysis of the characterization data, furfural adsorption mainly existed in η 1 (O)-aldehyde binding mode which was consistent with the density functional theory (DFT) calculation. DFT calculations of the reaction process showed that the theoretical results favored the hydrogenation of furfural through a hydroxyalkyl intermediate rather than of an alkoxide intermediate.
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Materials Today Communications
·
2023
·
IF 3.8
Sheng Dai,Luying Liu,Zhixing Wang,Huan Deng,Lei Zhou,JiaWei Cui,Zhaogui Su,Lizhu Xu,Li Yao,Ping Yang
Implanting vascular stents is regarded as a ground-breaking technique for treating cardiovascular disorders. Thus, advancements in vascular stent technology and stent materials have significant social and economic implications. The development of a surface with bionic endothelial function of nitric oxide (NO) release is always an ideal direction for cardiovascular material modification. However, The NO-release stents will face severe challenges in the oxidative stress microenvironment of atherosclerotic lesions. Excessive reactive oxygen species (ROS) can delay scaffold surface re-endothelialization by causing rapidly oxidative inactivation of NO and by causing endothelial cells (ECs) to undergo apoptosis. Regulating the oxidative stress microenvironment is crucial to address the aforementioned issues. In this study, a composite material that contains ultraviolet (UV)-modified and Copper (II) meso-tetra(4-carboxyphenyl) porphine (CuTPP)-loaded titanium dioxide nanotubes (NTs) was presented. CuTPP can efficiently catalyze the decomposition of ROS and also decompose GSNO into NO. As a unique technique, UV irradiation was used to enhance the anticoagulant properties of the CuTPP-loaded NTs ( [email protected] ). In vivo and in vitro results demonstrated that UV treated [email protected] maintained strong biocompatibility, anti-thrombosis, ECs and smooth muscle cells (SMCs) regulation, and anti-inflammatory capabilities. This technique might present a fresh idea for developing brand-new NO-release scaffolds.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yafei Qu,Wei Zheng,Peichen Wang,Hao Huang,Minxue Huang,Lin Hu,Hui Wang,Qianwang Chen
Electrochemical carbon dioxide reduction reaction (CO 2 RR) is an effective approach to capture CO 2 and convert it into value-added chemicals and fuels, thereby reducing excess CO 2 emissions. Recent reports have shown that copper-based catalysts exhibit excellent performance in converting CO 2 into multi-carbon compounds and hydrocarbons. However, the selectivity to the coupling products is poor. Therefore, tuning CO 2 -reduction selectivity toward C 2+ products over Cu-based catalyst is one of the most important issues in CO 2 RR. Herein, we prepare a nanosheet catalyst with interfaces of Cu 0 /Cu + . The catalyst achieves Faraday efficiency (FE) of C 2+ over 50% in a wide potential window between − 1.2 V to − 1.5 V versus reversible hydrogen electrode (vs. RHE). Moreover, the catalyst exhibits maximum FE of 44.5% and 58.9% towards C 2 H 4 and C 2+ , with a partial current density of 10.5 mA cm −2 at − 1.4 V. Density functional theory (DFT) calculations show that the interface of Cu 0 /Cu + facilitates C C coupling to form C 2+ products, while inhibits CO 2 conversion to C 1 products.
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