Nature Communications
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2025
·Vol. 16
·期 1
·1-12
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IF 15.7
Zhao Xin,Li Changzhi,Wen Jie,Qiang Qian,Shen Zirong,Yu Haipeng,Zhou Xin,Yue Fengxia,Fang Ruiqi,Li Yingwei,Zhang Tao
Lignin refining still suffers from great challenges of selective depolymerization and cleavage of stubborn C‒C linkages. Here, a robust atomically dispersed Cu/Ni-SA@HNC catalyst is fabricated for super-selective hydrogenolysis of lignin and model compounds via an unusual “preferential C α –C β bond cleavage in β-O-4 linkages” pathway, affording toluene in yield up to 75.7% from β-O-4 model compounds, and up to 33.7 ± 1.6 wt% (nine parallel experiments) from poplar lignin. The catalyst exhibits high stability, and the scale-up potential is demonstrated by the high space-time yield of toluene (33.7 g·g cat −1 ·h −1 ) in continuous flow reaction of β-O-4 model compound. The origin of the extraordinary selectivity towards C α –C β bond cleavage rather than C‒O bond cleavage in β-O-4 model compounds is uncovered. This work conquers the major challenges in lignin valorization by using non-noble dual-metal single-atom catalyst, not only showcasing the application perspective of atomically dispersed catalysts in biopolymer refinery, but also providing a cost-efficient, petroleum independent solution to valuable commodity chemicals.
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ACS Nano
·
2024
·
IF 15.8
Minglei Lu,Zhuoyu Zheng,Weiwei Lu,Haiping Zhu,Junwei Liao,Yuxin Ge,Xueer Huang,Qian Zhang,Jiajin Li,Yiyuan Zhou,Xiaoping Wu,Baozhu Chen,Chunxiao Yang,Xitang Qian,Minhua Shao,Tiejun Wang
Aqueous-phase reforming of methanol represents a promising avenue for hydrogen (H2) production. However, developing highly efficient and low-cost nonprecious catalysts remains challenging. Here, we report the synthesis of Cu-based catalysts with Cu, Cu2O, and CuN3 nanoparticles anchored on the nitrogen-doped carbon, forming Cu0/Cu+/Cu-N3 active sites. This catalyst achieves a H2 production rate of 140.1 μmol/gcat/s at 210 °C, which is several times to 2 orders of magnitude higher than that of Cu-, Ni-, even Pt-based catalysts, demonstrating excellent long-term stability over 350 h at 210 °C. A mechanism investigation reveals that the Cu-N3 site facilitates water dissociation into *OH and improves *CO and *OH conversion, leading to enhanced CO conversion and H2 production kinetics.
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Energy & Environmental Science
·
2024
·
IF 32.4
Liqun Wang,Jingting Jin,Wenzhi Li,Cunshuo Li,Leyu Zhu,Zheng Zhou,Lulu Zhang,Xia Zhang,Liang Yuan
Direct conversion of methane into high value-added products is of great practical significance. The synergistic effect in catalysts with dual-active components show potential to increase the methanol yield and selectivity. In this work, Cu–Pd/anatase is in situ generated and exhibits a relatively high methanol yield rate of ∼31 800 μmol gcat−1 h−1 and near-exclusive selectivity of liquid products (methanol). The reaction mechanism behind the heterogeneous catalysis process has been investigated. It is confirmed that copper ions hold the ability to produce hydrogen peroxide which can be further promoted by anatase. Chlorine ions can promote the stable adsorption of CO and the formation of *CH3 intermediates, facilitating high activity and selectivity for methanol production. Pd and Cu cooperatively dissociate methane, which promotes the formation of key configuration metal-CH3. The ˙CH3 intermediate desorption will be facilitated on Cu–Pd/anatase through the manner of electron regulation, which is proved by the combination of density functional theory calculations and in situ infrared spectroscopy. Methanol is formed when a ˙CH3 is desorbed from a copper site and combines with a hydroxyl radical.
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COMPOSITES COMMUNICATIONS
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2025
·
IF 7.7
Ke Zhang,Minghui Ou,Yujie Xiao,Zhiwei Wei,Li Yang,Yi Xie,Changsheng Zhao
Copper-based nanozymes have emerged as promising therapeutic agents for oxidative stress-related diseases due to their enzyme-mimicking properties. However, their development is still limited by poor biocompatibility, insufficient broad-spectrum free radical scavenging ability, and potential toxicity from Cu 2+ leakage. To address these challenges, we developed Cu@EA-BTC, a broad-spectrum antioxidant material, by integrating ellagic acid (EA) into copper-based metal-organic frameworks (Cu@BTC). The Cu@BTC serves as a stable copper source, while the EA endows the Cu@EA-BTC with broad-spectrum ROS scavenging and enhanced catalase (CAT)-like activity via facilitating the reduction of Cu 2+ to Cu + . As a result, the Cu@EA-BTC exhibits superior antioxidant properties and excellent biocompatibility, including both cellular and blood compatibility. Meanwhile, the Cu@EA-BTC effectively protects immune cells from oxidative damage, which indicates its potential for oxidative stress-related therapies. This study provides a promising strategy for developing safe and efficient nanozyme-based antioxidant materials for biomedical applications.
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JACS Au
·
2025
·
IF 8.7
Xuan Bie,Yukun Pan,Xiaowei Wang,Shiyu Zhang,Jiahui Hu,Xiaoxiao Yang,Qinghai Li,Yanguo Zhang,Robert E. Przekop,Yayun Zhang,Hui Zhou
Gas sources rich in CO2 derived from biomass/waste gasification, anaerobic digestion, or industrial carbon capture often contain impurities such as H2S, H2O, and NH3, which can significantly hinder catalyst performance. Here, we show the role of NH3 on the reverse water–gas shift (RWGS) reaction over a commercial Cu/ZnO/Al2O3 catalyst, examining its effects on both the catalytic activity and the catalyst structure. We found that NH3 reversibly decreases CO2 conversion immediately by suppressing carbonate hydrogenation and CO desorption. This effect intensifies with an increase in NH3 concentration but decreases at higher temperatures. However, prolonged exposure (over 100 h) to RWGS conditions in the presence of 1.4% NH3 leads to near-total and irreversible deactivation of the Cu/ZnO/Al2O3 catalyst. Under NH3 exposure, the catalyst loses Cu+ sites on the surface, causing a spatial separation of Cu and ZnO. Finally, to address this challenge, we propose a novel strategy to mitigate NH3 inhibition by decomposing NH3 into N2 and H2.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Chenxu Guo,Miao Li,Wenming Guo,Jiawei Xie,Hang Qin,Moyu Liao,Yi Zhang,Pengzhao Gao,Hanning Xiao
Methanol steam reforming (MSR) is considered as a promising approach to provide hydrogen for proton-exchange membrane fuel cells. However, it is challenging to develop effective and durable Cu-based catalysts. Herein, Cu-ZnO catalysts are prepared by facile quenching of ZnO in copper nitrate solution followed by reduction to obtain the desired metal loading and induce the doping of surface metal heteroatoms for producing more vacancies. Catalysts enriched with oxygen vacancies can efficiently activate H 2 O and rapidly transform C-containing intermediates, resulting in higher methanol conversion and lower CO selectivity. As a result, the quenched optimal catalyst achieves 100 % methanol conversion and 0.05 % CO selectivity at 280 ℃, exhibiting the excellent catalytic performance in MSR reaction. In practical applications, structured catalysts are more attractive for large-scale catalytic reactions owing to the low pressure drop and high utilization efficiency. Therefore, ZnO-Cu 3 catalyst is coated on cordierite honeycomb ceramics with 100 % methanol conversion and 0.04 % CO selectivity at 280 ℃. After 100 h of the reaction, the structured catalyst remains ∼ 92.3 % with CO selectivity varying from 0.02 to 0.06 %, demonstrating the good catalytic stability in the long-term experiment. In addition, the evolution of reactants and intermediates on the catalyst surface are briefly described by FTIR spectra. This study offers a novel and efficient approach to obtain highly active and durable catalysts with great potential for industrial-scale preparation and application.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Haitao Yan,Didi Li,Zhaocong Jiang,Haoyuan Gu,Mengyuan Zhu,Yi-Fan Han,Minghui Zhu
Cu-based catalysts have been extensively used in the methanol steam reforming (MSR) reaction owing to low cost and high efficiency. In this work, we investigated the promotional effect of Fe on the Cu/ZnO/Al 2 O 3 catalysts prepared by an incipient-wetness impregnation method using a series of (quasi) in situ characterization techniques. The form of the Fe species was found to strongly depend on the Fe content. Fe species are present as highly dispersed FeO x in small amount of Fe with improved the dispersion of Cu. As Fe content increases, Fe species gradually transition to CuFe alloy and eventually to Fe 3 O 4 particles, leading to a decrease in Cu dispersion. With the gradual increase in Fe content, the apparent activity shows a volcanic trend, with CuAl-0.1Fe showing highest activity, whereas the intrinsic activity gradually decreases. Compared with CuAl- x Fe, adding moderate Fe to Cu/ZnO/Al 2 O 3 promotes the dispersion of Cu and Zn, forming abundant Cu-ZnO x interfacial sites, which improves both apparent and intrinsic activities. The best catalytic performance was obtained with the CuZnAl-0.1Fe catalyst, achieving the highest H 2 production rate of 134.7 mmol g cat −1 h −1 at 200 °C. This study reveals the role of Fe in Cu-based catalysts for MSR and inspires the design of improved Cu-based catalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Qian Liu,Wenqian Luan,Xingrong Zhang,Ruiyang Zhao,Jishu Han,Lei Wang
The design of a low-cost, efficient and durable co-catalyst for hydrogen evolution is of great significance for improving photocatalytic activity. In this work, a NiMoP 2 /Cu-ZnS composite photocatalyst was prepared by in-situ growth of NiMoP 2 on the surface of copper-doped zinc sulfide (Cu-ZnS). The test results showed that the hydrogen production rate of the optimized NiMoP 2 /Cu-ZnS under visible light irradiation was significantly improved. Among them, NiMoP 2 /Cu-ZnS-1 exhibited the highest photocatalytic activity (5.13 mmol·g −1 ·h −1 ), which was 2.47 times that of Cu-ZnS and maintained good stability during the reaction. The improvement of hydrogen production performance of the photocatalyst was mainly attributed to the synergistic effect of Cu-ZnS and co-catalyst NiMoP 2 . The ohmic contact formed between Cu-ZnS and NiMoP 2 could improve the separation efficiency of photogenerated carriers and reduce the overpotential of H 2 evolution. Besides, NiMoP 2 was found to provide the active site for the reduction reaction, and accelerate the transfer efficiency of photogenerated electrons. This strategy opens up a new way for the construction of co-catalyst modified semiconductor materials to improve the photocatalytic hydrogen production rate.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2013
·
IF 1.977
Yu Ling,Na Zhang,Fei Qu,Ting Wen,Zhong Feng Gao,Nian Bing Li,Hong Qun Luo
An interesting, simple, and label-free strategy for the detection of hydrogen peroxide and glucose has been developed with polyethyleneimine (PEI)-capped copper nanoclusters as a fluorescence probe in aqueous solution. The PEI-templated Cu nanoclusters which we have synthesized have an average diameter of 1.8 nm and show a blue emission at 480 nm. In the presence of hydrogen peroxide, the fluorescence of the Cu nanoclusters is quenched. Similarly, glucose oxidase catalyzes the oxidation of glucose to gluconic acid and H 2 O 2 , so we can also use this probe to detect glucose. Because of the high zymolyte specificity of glucose oxidase, the detection of glucose has good selectivity. Under the optimized experimental conditions, the linear ranges for H 2 O 2 and glucose are 0.5–10 μM and 10–100 μM, respectively. And the detection limits for H 2 O 2 and glucose are 0.4 and 8 μM, respectively. Furthermore, we discussed the mechanism of fluorescence quenching which is caused by the interaction between H 2 O 2 and Cu nanoclusters. This sensing system has been applied successfully to the detection of glucose in human serum samples.
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Nano Research
·
2021
·Vol. 14
·期 8
·2831-2836
·
IF 8.897
Mou Shiyong,Li Yonghao,Yue Luchao,Liang Jie,Luo Yonglan,Liu Qian,Li Tingshuai,Lu Siyu,Asiri Abdullah M.,Xiong Xiaoli,Ma Dongwei,Sun Xuping
The advancement of cost-effective and selective electrocatalyst towards CO 2 to CO conversion is crucial for renewable energy conversion and storage, thus to achieve carbon-neutral cycle in a sustainable manner. In this communication, we report that Cu 2 Sb decorated Cu nanowire arrays on Cu foil act as a highly active and selective electrocatalyst for CO 2 to CO conversion. In CO 2 -saturated 0.1 M KHCO 3 , it achieves a high Faraday efficiency (FE) of 86.5% for CO, at −0.90 V vs. reversible hydrogen electrode (RHE). The H 2 /CO ratio is tunable from 0.08:1 to 5.9:1 by adjusting the potential. It is worth noting that HCOO − product was totally suppressed on such catalyst, compared with Sb counterpart. The improving selectivity for CO could be attributed to the bimetallic effect and nanowire arrays structure.
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MATERIALS CHEMISTRY AND PHYSICS
·
2019
·
IF 2.781
Zhiqiang Xu,Xianhua He,Mingwei Liang,Lijuan Sun,Di Li,Kenan Xie,Li Liao
Catalytic reduction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) over high-performance non-noble metal catalysts is attracting intensive attention. Herein, we report a graphene supported Cu@Ni bimetallic nanowires catalyst by a facile liquid phase reduction method with the assistance of an external magnetic field. The morphology and structure of the composite are studied by SEM, TEM and XPS. The vibrating sample magnetometer (VSM) is used to analyze its magnetic properties . Owing to the synergistic effect of graphene and bimetallic nanowires, the catalyst shows superior catalytic performance and excellent stability. The results of catalysis exhibit an extraordinary rate constant (1.16 min −1 ) and activity factor (5.81 min −1 mg −1 ) at room temperature, which are much higher than a majority of non-noble metal catalysts, even noble metal catalysts. Also, compared with noble metal catalyst, the novel catalyst possesses ferromagnetism , which facilitates the separation of catalyst and reaction system, and guarantees recyclability. Moreover, a possible synergistic catalytic mechanism based on the fact that electron transfer between copper-nickel nanowires and graphene has been proposed. It is believed that the novel catalyst has a great importance for the application of nanowires in the field of catalysis.
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JOURNAL OF CATALYSIS
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2021
·
IF 7.92
L.J. Zhang,J.C. Yuan,L.J. Ma,Z.Y. Tang,X.M. Zhang
Zirconium-based porphyrinic MOFs (PMOFs, MOF = metal-organic framework) have gained considerable attention in the field of electric/thermo/photo-catalysis as heterogeneous single-site catalysts; however, the study on multisite synergistic catalysis of PMOFs are rare. Herein, we have successfully developed a highly regio- and stereo-selective synthetic method of ( E )- β -vinylboronates through hydroboration of alkynes using PCN-222 (Cu, PCN = porous coordination network) as multifunctional heterogeneous catalyst. Compared with homogeneous catalytic system, high TOF value is achieved in the developed method, originating from the synergistic effect of central Cu(II) ions, N atoms of porphyrin rings and terminal –OH groups on Zr-nodes. Notably, density functional theory (DFT) study reveals that five-membered “Cu-N-B-C-C” ring is the key species responsible for the hydroboration process with specific selectivity.
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