Catalysis Science & Technology
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2022
·Vol. 12
·期 19
·5879-5890
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IF 6.177
Dengfeng Dai,Chao Feng,Minmin Wang,Qingzhou Du,Dandan Liu,Yuan Pan,Yunqi Liu
Biomass-based chemicals as a renewable alternative to petroleum-based chemicals are of great significance. The conversion of biomass-based furfuryl alcohol to pentanediol, including 1,5-pentanediol and 1,2-pentanediol, is explored over a series of bifunctional Cu/MFI catalysts in a continuous-flow reactor. These catalysts are synthesized by supporting copper nanoparticles on MFI zeolites with varying molar ratios of SiO2/Al2O3. Among them, the Z60-10Cu catalyst containing balanced Cu0–Cu+ and Brønsted acid sites exhibits excellent performance, and a high furfuryl alcohol conversion of 99.5% and selectivity of 85.2% for 1,5-pentanediol (69.2%) and 1,2-pentanediol (16.0%) could be achieved (hydrogen pressure: 2.5 MPa) at 160 °C. The experimental results and the results obtained using the DFT technique revealed that the high catalytic activity realized during the processes of ring-opening and hydrogenation could be attributed to the synergistic effect between the Cu species and Brønsted acid sites. The Brønsted acid sites on the Si(OH)Al groups significantly affect the ring-opening process of furfuryl alcohol. The methoxy group on furfuryl alcohol adsorbs on the Cu+ sites, and the hydrogenation saturation of the ring-opening intermediate is realized under the influence of the activated hydrogen units on the Cu0 sites. The results reported herein could help promote the continuous production of high value-added pentanediol from biomass-based raw materials in the presence of non-noble metal catalysts. An economical and feasible path for the transformation of biomass resources into high value-added fine chemicals could also be developed.
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JOURNAL OF HAZARDOUS MATERIALS
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2026
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IF 10.6
Dingqiang Zhang,Xiaoqun Wu,Tengchao Jiao,Weizhen Zhang,Jiahao He,Yanhua Xie,Yingming Hu,Yao Wei
Trace-Cu(II)/CaO 2 /PAC achieves > 95% algal removal in natural waters. • Pre-oxidation degrades algal extracellular matter to aid coagulation. • PAC mitigates matrix interference, indirectly maintaining oxidation. • Intracellular ROS induces functional death without severe lysis. Harmful algal blooms release microcystins and other metabolites that threaten aquatic ecosystems and human health. Conventional removal methods often induce cell lysis and are affected by matrix interference in natural waters, limiting their practical applicability. A sequential process coupling trace-Cu(II)/CaO 2 pre-oxidation with PAC coagulation was developed for efficient algal removal. The system removed 98.5% of M. aeruginosa from lake water. During the 10-min pre-oxidation stage, trace-Cu(II)/CaO 2 effectively degraded extracellular microcystin-LR (MC-LR) and the dissolved organic matter (DOM) surrounding algal cells, thereby weakening electrostatic repulsion and enhancing coagulation efficiency. The coupled process generated Cu(III), •OH, •O 2 − , and 1 O 2 within the cells, which led to functional cell death without severe membrane rupture. Conventional molecular dynamics (MD) simulations confirmed the stability of a representative pentameric cation-channel model, and steered molecular dynamics (SMD) further showed that Cu 2+ and H 2 O 2 could be guided through its pore under an applied axial bias, supporting the physical plausibility of channel-mediated intracellular access. Mechanistically, OH − generated during CaO 2 hydrolysis promoted the Cu(II)/Cu(I)/Cu(III) catalytic cycle and sustained reactive species production, with Cu(III) as the dominant contributor to functional inactivation (68.5%). These findings establish an innovative and practical strategy for the safe and effective removal of algae from contaminated natural waters. Download: Download high-res image (297KB) Download: Download full-size image
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Nanoscale
·
2018
·Vol. 10
·期 37
·17647-17655
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IF 7.233
Ke Yang,Yu Yan,Haiyang Wang,Zhixuan Sun,Wen Chen,Hongtao Kang,Yi Han,Wenquan Zahng,Xiaohua Sun,Zhenxing Li
A novel copper/copper(I) oxide@carbon (Cu/Cu2O@C) core–shell nanocomposite monodispersed on the surface of reduced graphene oxide (defined as Cu/Cu2O@C-rGO) was synthesized using a one-step calcination of Cu-based metal organic frameworks (MOFs)/graphene oxide (GO) composite structure. The size of the resultant Cu/Cu2O@C core–shell nanoparticles (NPs) on the rGO layers were mainly distributed in range of about 90–100 nm with good dispersion, which was characterized using transmission electron microscopy. X-ray diffraction, Raman spectroscopy, Fourier transform infrared spectroscopy, nitrogen adsorption–desorption isotherms, X-ray photoelectron spectrometry and thermogravimetric analyses were also carried out to characterize the structure and composition of the Cu/Cu2O@C-rGO. The catalytic performance of the Cu/Cu2O@C-rGO composite was evaluated using a reduction reaction from 4-nitrophenol to 4-aminophenol. It was demonstrated that the Cu/Cu2O@C-rGO composite exhibited an excellent catalytic performance, which can reach a nearly 100% conversion rate in 90 s with 0.1 mg of catalyst. This catalyst also showed a good performance for the degradation of other organic dyes such as methylene blue, methyl orange and rhodamine B. Additionally, the core–shell structure exhibited good stability and reusability for the reduction reaction, which was because of its relatively better oxidation resistance than that of the bare Cu NPs. This research provided an efficient and stable non-noble metal-based catalyst derived from the MOF/GO structure.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Fuxia Huang,Zihao Jiao,Feng Wang,Ya Liu,Liejin Guo
Direct photocatalytic CO 2 conversion to C 2 products holds notable potential, but this technology is still limited by the high thermodynamic energy and sluggish kinetics. By introducing Cu in In 4 SnS 8 catalyst, we here developed low S vacancies and chemical reactive sites photocatalysts Cu-In 4 SnS 8 , enabling photocatalytic CO 2 to ethanol with full selectivity. Minor electron paramagnetic resonance peak intensity and large formation energy for S-vacancy suggest Cu introduction suppresses S vacancies formation. Low S vacancies photocatalysts Cu-In 4 SnS 8 possess excellent carrier transfer and separation ability by the steady photoluminescence and transient fluorescence characteristic results. Furthermore, in situ, FTIR measurements confirmed ethanol formation via the presence of the intermediates *COOH, *CO, *OCCO(H), and *OCH 2 CH 3 . Also, theory calculations reveal that Cu efficiently reduces the energy barriers of the rate-limiting steps of *COOH and *COH, and promotes C-C coupling and multi-proton coupled electron transfer processes by co-adsorption and asymmetric charge distribution effects. As a result, the optimized sample achieves 0.73 μmol h −1 CH 3 CH 2 OH generation with full selectivity.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
·
IF 8.1
Lu Li,Shiyu Ma,Huimin Liu,Zixuan Zeng,Qijie Li,Chunlin Song,Jingang Yang
Ammonia borane (NH 3 BH 3 ) as a solid chemical hydrogen storage material with a high hydrogen content can be hydrolyzed under mild conditions to release hydrogen. In this work, Fe–Ni–B/Cu(OH) 2 –Cu foam was synthesized by combining in situ growth and electroless plating. Compared with the binary Fe–B/Cu(OH) 2 –Cu foam and Ni–B/Cu(OH) 2 –Cu foam prepared by the same method, the ternary Fe–Ni–B/Cu(OH) 2 –Cu foam has superior catalytic performance. The Fe–Ni–B/Cu(OH) 2 –Cu foam catalyst was able to achieve a maximum hydrogen production rate of 5.6 ml min −1 cm −2 at 298 K with an activation energy as low as 46.3 kJ mol −1 . And more importantly, its catalytic efficiency has hardly decayed after ten cycles. These excellent properties are due to its low activation energy and the large specific surface, multi–site Cu(OH) 2 –Cu–foam carrier.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Xuli Hu,Zhen Zhang,Zhenyao Li,Yushan Wu,Wei Wei,Yao Wang,Junchen Xu,Mingyue Ding
Regulating oxidation state of Cu-based chalcogenides catalysts during electrolysis is of great significance for efficient CO 2 electrochemical reduction reaction (CO 2 RR) to methanol, which still remains a dramatic challenge. Herein, we construct a heterogeneous Cu 3 VS 4 /CuS electrocatalyst (denoted as CuV x S), in which the in-situ growing Cu-S-V bonds avoid the accumulated electrons on oxidized Cu sites and inhibit the deep reduction of CuS to metallic Cu during electrolysis, maintaining stable and abundant reactive Cu + /Cu 2+ species to promote CO 2 RR performance to methanol. By this design, the CuV 0.1 S catalyst achieves an ultrahigh methanol selectivity of 79.8 %. In-situ FTIR measurement reveals that the synergistic effect of Cu + /Cu 2+ species and Cu-S-V bonding facilitates the *CO adsorption and the subsequent *CO hydrogenation process, which improve the generation of *CHO and *OCH 3 intermediates for enhanced methanol selectivity. This work provides a new insight into stabilizing high oxidation state of Cu-based electrocatalyst to maintain sufficient active sites for CO 2 RR.
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Materials Today Communications
·
2025
·
IF 4.5
Peibo Li,Guoqiang Luo,Guinan Zhao,Yi Sun,Qiang Shen
The scale effect of intermetallic compounds (IMCs) plays a pivotal role in governing the mechanical behavior of Al-Cu composites. To investigate this, a series of composites incorporating intermetallic compounds (IMCs) of varying dimensions was fabricated. Experimental results reveal that the mismatch in thermal expansion coefficients between the IMCs and the Al matrix induces interfacial strain gradients. At the nanoscale, these gradients facilitate the nucleation of fault networks that effectively impede dislocation motion by reducing the mean free path, thereby surpassing the limitations predicted by the conventional Hall–Petch relationship. Moreover, nanoscale IMCs serve as dislocation pinning sites, thereby activating the Orowan strengthening mechanism. In contrast, micron-scale IMCs demonstrate limited ability to form dislocation loops, and the stacking faults (SFs) generated during stress relaxation become sources of mobile dislocations. The acceleration of dislocation at phase boundaries leads to stress concentration and premature failure. These insights provide valuable guidance for the structural and compositional design of metal matrix composites .
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Journal of Materials Chemistry A
·
2026
·
IF 9.2
Guangbo Wang,Hao Zhang,Jiahao Yang,Zeyi Lu,Wenqiong Li,Yanmei Tang,Yun He,Xiaoguang Liang,Xingyuan San,Vellaisamy A. L. Roy
In the quest to optimise the catalytic activity and selectivity of the CO2 reduction reaction (CO2 RR), various imperfections-such as defects, grain boundaries, and vacancies-pose significant challenges. In a groundbreaking approach, we present the synthesis of well-structured CuAl nanocrystals featuring a preferential (111) crystal facet, a first in the field. This innovative structure not only enhances selectivity but also establishes a clear structure-activity relationship for CO2 RR. The unique properties of CuAl nanocrystals stem from their ability to finely control bonding interactions with CO2 RR intermediates, driven by the synergistic effects of the (111) facet. Utilising a straightforward chemical vapour deposition (CVD) method, we produce these nanocrystals, revealing the atomic distribution of Cu and Al on this dominant surface, which crucially influences CO2 RR performance. Among them, Cu96Al4 achieves the highest Faraday efficiency (FE) for HCOOH (77.71%) and CO (18.01%), attributed to the synergistic effects of Cu and Al arising from the optimal d-band centre of Cu active sites and the strong electron-donating ability of Al. This interaction facilitates the electron transfer from Cu to *COOH, resulting in a high FE for C1 product. Our findings pave the way for advanced catalytic designs that can significantly elevate CO2 conversion efficiencies.
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ACTA PHYSICO-CHIMICA SINICA
·
2026
·
IF 13.5
Miao Zhao,Qi Mao,Pengfei Zhang,Manyi Gao,Xuefei Zhao,Chunmei Ding,Can Li
With the advancement of industry and agriculture, substantial nitrate-containing pollutants have been discharged. This leads to severe environmental pollution and imbalance in nitrogen cycle, threatening ecology environment and human health. Electrocatalytic nitrate reduction to ammonia can convert pollutants into important chemical feedstocks and energy-storage molecules, providing a feasible route for ammonia production using renewable energy. However, this reaction is complicated and involves multiple steps and intermediates, suffering from high overpotential and limited selectivity and activity. To solve this issue, herein we designed a mixed-valence Cu/CuO x catalyst which is primarily composed of Cu and Cu 2 O and shows three-dimensional nanowire structure, achieving efficient nitrate reduction reaction for ammonia synthesis. The current density for ammonia production reaches 1.89 A·cm −2 at −0.22 V vs . RHE (reversible hydrogen electrode), with a Faradaic efficiency of 80.9%. Cu/CuO x also maintains excellent stability during prolonged electrolysis. The apparent and normalized performances of Cu/CuO x are much higher than those of the control systems, such as Cu and Cu 2 O. Experimental and theoretical results prove that the Cu 0 and Cu + species in Cu/CuO x play synergistic roles, promoting the conversion of *NO intermediate to *NOH and accelerating the desorption of NH 3 . The nanowire structure provides abundant active sites, thereby enhancing the performance of nitrate reduction to ammonia. This work not only provides an efficient catalyst for nitrate reduction to ammonia but also serves as a guideline for the rational design of such catalysts. Synergistic effect of Cu 0 and Cu + in Cu/CuO x nanowires enables efficient nitrate reduction to ammonia. Download: Download high-res image (261KB) Download: Download full-size image
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Green Energy & Environment
·
2026
·
IF 16.7
Yusi Wang,Hui Zhang,Daolan Liu,Yanfei Zhao,Wei Zeng,Rongxiang Li,Minhao Tang,Yuxuan Wang,Xianshuo Zhang,Zhimin Liu
The recycling of spent polyesters into oxygen-containing chemicals provides a novel way to access such chemicals, and is also of great significance for solving the problems caused by polyester waste. Herein, we present hydrogenolysis of aliphatic polyesters into diols over MgAlO x supported Cu catalysts (Cu/MgAlO x -m) via a methanolysis-hydrogenation strategy under relatively mild conditions (e.g., 200 °C, 4 MPa). The as-designed Cu/MgAlO x -10 catalyst with Cu content of 10 wt.% shows the best performance, which could convert polycaprolactone into 1,6-hexanediol in a high yield of 98.0%. It is revealed that the Cu species in the catalyst mainly exist in the form of Cu 0 and Cu + , in which Cu 0 is responsible for H 2 activation, and Cu + for ester group activation and stabilization of reactive intermediates. The ratio of Cu 0 to Cu + species determines the selectivity towards diols. This work provides a highly efficient catalyst for hydrogenolysis of aliphatic polyesters into diols, which may have industrial application prospects.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Hanjun Zou,Yan Tong,Yajie Feng,Yongfeng Zhou,Jiaxun Xiao,Lu Xia,Anku Guha,Barbara Polesso,Bin Zhang,Juanli Liu,Kaiwen Wang
Subnanocluster (SNC) cocatalysts are considered to be promising cocatalysts for photocatalytic hydrogen evolution reaction (HER) due to their rich surface-active sites and high atom utilization efficiency. Herein, a reductant-mediated in situ growth of the atomic clusters procedure is developed to synthesize SNC-Cu serving as advanced cocatalysts on TiO2 nanoparticles for HER. The optimized SNC-Cu/TiO2 catalyst, with 1.8 wt % metal mass loading, exhibits a remarkable hydrogen evolution rate of 6832 μmol g–1 h–1, which is ca. 25-fold that of bare TiO2 (273 μmol g–1 h–1 and comparable to that of 1 wt % Pt-modified TiO2 (7754 μmol g–1 h–1). Meanwhile, decent photostability and recyclability are also certified via a 20 h durability test. Comprehensive electron microscopy and spectroscopy characterizations unveil that the outstanding performance of SNC-Cu/TiO2 can be attributed to accelerated charge separation/transfer and suppressed photoinduced electron–hole recombination. Furthermore, in situ X-ray photoelectron spectroscopy and first-principle calculations reveal that the electron-localized SNC-Cu, with its abundant surface sites, facilitates *H adsorption and desorption, thus enhancing the HER activity significantly. This work highlights the promising potential of constructing noble-metal-free SNCs in semiconductors for photocatalytic HER.
研究领域:
材料科学
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能源科学
·
化学
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PHOSPHORUS SULFUR AND SILICON AND THE RELATED ELEMENTS
·
2022
·
IF 1.052
Xin Zhang,Liang Wang,Qiaoyong Zhu
A chlorosulfonylation of vinylarenes using magnetic metal–organic framework (MOF) composite Cu-BTC@Fe3O4 (BTC = 1,3,5-benzenetricarboxylate) as the catalyst has been developed. This protocol features easily accessible starting materials, good functional group compatibility and simple recovery of the catalyst. The recovered catalyst could be reused for at least successive five runs with only a slight decrease in its catalytic activity.
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