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.
研究领域:
电化学
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催化材料科学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF MODERN PHYSICS B
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2017
·
IF 0.736
Hongcheng Peng,Weihong Qi,Wenhai Ji,Siqi Li,Jieting He
Combining the bond-energy model and Debye theory, we generalized the Gibbs free energy model for Cu–Pt nanoparticles (NPs) by introducing a shape factor considering the shape effect. We studied the structural stability of the Cu–Pt NPs and plotted the corresponding composition-, shape- and size-dependent phase diagrams. It is shown that the Cu–Pt NPs can form alloyed structure in a large size range. But when the particle size continues to decrease, the NPs will form the core–shell structure due to surface segregation. Meanwhile, the composition segregation could make the atoms of less-content element to gather in the surface. The predictions from the present calculated phase diagrams are consistent with a series of experimental results in literatures. To further prove the efficiency of the phase diagrams, we synthesized the alloyed Cu–Pt NPs of 4–15 nm by a co-reduction method, which is in agreement with the predictions from the phase diagrams.
研究领域:
材料科学
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纳米技术
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DOI
高影响因子
CATALYSIS COMMUNICATIONS
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2024
·
IF 3.4
Yu Sun,Jinxing Mi,Liang Li,Shuxiu Yu,Shixiong Yuan,Guimin Wang,Jianjun Chen,Junhua Li
The unique ability of Cu + to enhance C-C coupling makes it important in the field of CO 2 reduction reaction (CO 2 RR) over Cu-based catalyst, while Cu + is very prone to deactivation. Hereby, we propose a simple and feasible stabilization strategy to stabilize Cu + species through reducing Cu-Mg-Al hydrotalcite by adding ascorbic acid, which owns stable product selectivity in a span of 6 h at −0.95 V vs.RHE. Characterization results show that the excellent stability is promoted by the heterostructure of Cu 2 O and hydrotalcite with retained Cu + species, which derives from Cu 2 O and slow down the rapid reduction of Cu + to Cu 0 .
研究领域:
材料科学
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电化学
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环境科学
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产品关联
DOI
高影响因子
VACUUM
·
2024
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IF 3.8
Xiu Wen,Zhixiu Yang,Lijing Gao,Ruiping Wei,Xiaomei Pan,Jin Zhang,Guomin Xiao
Electrocatalytic reduction of CO 2 affords a potential way to mitigate the greenhouse effect and fuel crisis. In this work, we compared highly-dispersed CuO nanocomposites and Cu–Cu 2 O nanocomposites which all derived from Cu x Al-LDH for CO 2 electrochemical reduction . The Cu–Cu 2 O based nanocomposites obtained through the restoration strategies still retain its layered structure, simultaneously increasing dual Cu–Cu 2 O active sites, which exhibit excellent performance in selective reduction of CO 2 to C 2 H 4 . The Cu 5 Al-ER obtained through in-situ electrochemical reduction is modified by bulk phase, which can regulate active species, increase surface active sites, enhance C–C coupling. Meanwhile, the electrochemical strategy offers numerous benefits, including gentle conditions, adjustable monitoring, exceptional efficiency and adaptability. We have confirmed that cost-effective Cu–Cu 2 O based nanocomposite derived from Cu 5 Al-LDH can effectively promote C–C coupling during electrochemical CO 2 conversion and improve FE C2H4 . The FE C2H4 of Cu 5 Al-ER reaches 36% at −1.2 V vs. RHE. And the current density reaches −172 mA·cm −2 at −1.6 V vs. RHE. The results showed that compared to Cu 5 Al-LDO, the FE C2H4 of Cu 5 Al-ER increased by 2.6 times. In addition, Cu 5 Al-ER exhibits excellent stability during the 12 hours CO 2 catalytic reduction process.
研究领域:
化学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL PHYSICS LETTERS
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2024
·
IF 2.8
Ye Liu,Lei Zhang,Yubo Kuang,Xiaoqian Xiang,Haohan Tao,Guangran Di,Xiaojing Yin,Meicheng Li,Xiao-Jun Lv
The photocatalytic CO 2 reduction has the problems of low selectivity of single product. Here, the preparation of Cu modified tubular C 3 N 4 (CTN) was studied. The increase of the active site inhibits the recombination of electrons (e-) and holes (h + ) and improves the selectivity of CO 2 reduction products. Finally, the CO and CH 4 yields of 1.5 % CTN photocatalyst are 11.55 μmol·g −1 and 4.72 μmol·g −1 , respectively, which are 5 times higher than that of tubular C 3 N 4 photocatalyst. The selectivity of 2 % CTN to CH 4 is up to 68 %, indicating that the prepared CTN photocatalyst has high CO 2 reduction activity and CH 4 selectivity.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2018
·
IF 4.521
Shaozhong Li,Yu Wang,Bin Yang,Limin Guo
Mesostructured catalysts with optimized microstructure and surface properties endowed them attractive catalytic performance. Herein, the mesostructured AlCeO supports with different weight ratio of Al 2 O 3 and CeO 2 have been prepared on the basis of a self-assembly sol-gel process, then 15 wt.% Cu was loaded onto the mesostructured AlCeO supports by incipient wetness impregnation method. The mesostructured AlCeO supports with varied ratio of Al 2 O 3 to CeO 2 resulted in the very different Cu particle size, and for the optimized catalyst Cu/AlCeO-7 (the amount of Al 2 O 3 in AlCeO support was 70 wt.%), the Cu crystal size was around 7 nm based on the characterization of XRD and TEM. The Cu/AlCeO-7 catalyst had strong metal-support interactions (SMSI) and more Cu-ceria interface, which was confirmed by the XPS. Furthermore, the Cu/AlCeO-7 catalyst showed the highest exposed Cu surface area ( S Cu ) (25.5 m 2 /g cat ) from the analysis results of H 2 -TPR and dissociative chemisorption of nitrous oxide. The CO 2 -TPD results demonstrated the Cu/AlCeO-7 had strong surface basicity. Hence, Cu/AlCeO-7 catalyst showed the highest space time yield of methanol (STY MeOH ). The CO 2 conversion (Cu/AlCeO-7, V(H 2 )/V(CO 2 ) = 3/1, GHSV = 6000 mL h −1 g −1 and P = 4 MPa) was up to 22.5% at 553 K, the methanol selectivity can reach 94% at 473 K, and the STY MeOH was up to 7.2 mmol g cat. -1 h -1 at 493 K. The as-prepared mesostructured Cu/AlCeO-7 exhibited a promising catalyst candidate for CO 2 hydrogenation to methanol.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Yufang Wu,Zhenqiang Lv,Xin Zhou,Junjie Peng,Yuning Tang,Zhong Li
We report a bifunctional SBU-tuning strategy that simultaneously enhances the selective CO 2 adsorption capacity of Cu-BTC and its structural stability under moisture. A series of Gly@Cu-BTCs were prepared by grafting glycine (Gly) to the secondary building units (SBUs) of the commercially available Cu-BTC through the nano-seed assistant ultrafast room temperature synthesis. N 2 isotherms evidenced higher BET specific surface area and pore volume of Gly@Cu-BTCs than that of Cu-BTC. Hence, Gly 0.3 @Cu-BTC exhibited a superior CO 2 capacity of 5.4 mmol/g at ambient conditions, which is 12% higher than that of Cu-BTC. Besides, the adsorptive selectivity of Gly 0.3 @Cu-BTC for the equimolar CO 2 /CH 4 and CO 2 /N 2 mixtures was separately up to 8.53 and 59.38, being 11% and 15% higher compared to that of Cu-BTC. More importantly, the stability of Gly 0.3 @Cu-BTC against moisture was improved. After 10 days’ exposure in 55% relative humidity, Gly 0.3 @Cu-BTC preserved 80% of its original CO 2 capacity, while only 9% CO 2 capacity remained for Cu-BTC. In addition, negligible CO 2 capacity loss of Gly 0.3 @Cu-BTC was observed in the subsequent 10 days in moisture after the initial exposure. Gly 0.3 @Cu-BTC exhibited excellent regenerability, and its CO 2 desorption efficiency reached up to 98% based on the consecutive adsorption-desorption cycles. The origination of the improved stability under moist of Gly 0.3 @Cu-BTC was interpreted with DFT calculation. The bifunctional SBU-tuning strategy demonstrated in this work enables the potential adsorptive separation application of Cu-BTC under moist working condition.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
iScience
·
2025
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IF 4.1
Hong Qian,Binxia Yuan,Yuhao Liu,Li Wang,Rui Zhu,Pengyu Dong
TiO 2 has low photocatalytic activity due to its easy recombination of photogenerated charges and low visible light utilization efficiency. This study utilized the keto-enol tautomerism principle of fructose in an alkaline environment to successfully obtain Cu 2 O/TiO 2 (CT), Cu 2 O/TiO 2 /Cu (CTC), and TiO 2 /Cu (TC) catalysts. As Cu(I) transformed into Cu(0), the bandgap narrowed, significantly enhancing visible light absorption. Photocatalytic tests showed that CT-0.15 exhibited the highest hydrogen production rate (279.53 μmol g −1 h −1 ), which was 25.18 times higher than that of TC-2. However, CTC-1 had the highest CO production rate (10.58 μmol g −1 h −1 ). Optoelectronic test revealed that CT-0.15 and CTC-1 had higher separation efficiency of photogenerated exciton. Density functional theory (DFT) calculations indicated that the change in the valence state of Cu influenced the reaction mechanism, with CT being favorable for the adsorption of H + in HER and CTC promoting the adsorption of CO 2 in carbon dioxide reduction reaction (CO2RR).
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Catalysts
·
2019
·Vol. 9
·期 6
·538
·
IF 3.444
Lili Liu,Xiaojing Zhou,Li Liu,Shuai Jiang,Yingjie Li,Luxia Guo,Shijuan Yan,Xishi Tai
Three bimetallic Cu–Ni nanoparticle-supported catalysts were synthesized by co-immobilization followed by H2reduction. A chromium(III) terephthalate metal organic framework (MIL-101), titanium dioxide (TiO2), and carbon (C) with different properties (acidity and Brunauer–Emmett–Teller surface area) were selected as supports for studying the effect of the support nature on the catalytic activity and selectivity in the oxidation of benzyl alcohol. The physicochemical properties of the Cu–Ni-supported catalysts were characterized by XRD, NH3-TPD, nitrogen adsorption/desorption, TEM, EDS, XPS, and ICP-OES. Bimetallic Cu–Ni nanoparticles were highly dispersed on the support. The catalytic activities of CuNi/MIL-101, CuNi/TiO2, and CuNi/C were tested in the selective oxidation of benzyl alcohol to benzaldehyde in the presence of molecular oxygen under mild reaction conditions. The highest benzaldehyde yields were achieved with CuNi/TiO2, CuNi/MIL-101, and CuNi/C catalysts at 100 °C within 4 h under 5, 3, and 3 bar of O2, respectively. The bimetallic Cu–Ni-supported catalysts possessed two types of catalytic active sites: acid sites and bimetallic Cu–Ni nanoparticles. The CuNi/MIL-101 catalyst possessed a high number of acid sites and exhibited high yield during selective benzyl alcohol oxidation to benzaldehyde. Importantly, the catalysts exhibited a high functional group (electron-donating and electron-withdrawing groups) tolerance. Cu–Ni-supported catalysts with an Cu:Ni mole ratio of 1:1 exhibited the highest yield of 47% for the selective oxidation of benzyl alcohol to benzaldehyde. Reusability and leaching experiment results exhibited that CuNi/MIL-101 showed better stability than CuNi/TiO2and CuNi/C catalysts due to the large porous cavities of MIL-101 support; these cavities can be used to trap bimetallic Cu–Ni nanoparticles and inhibit nanoparticle leaching.Keywords:Cu–Ni nanoparticles;MIL-101;TiO2;carbon;benzyl alcohol oxidation
研究领域:
催化
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2025
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IF 13.1
Jia-qi Bai,Mei Ma,Huangfei Liu,Zhangkai Qian,Durui Liu,Yuncai Zhao,Yijing Gao,Jingshuai Chen,Mengdie Cai,Song Sun
The hydrogenation of nitriles is an environmentally friendly and atom-economical route to prepare high-value amines; however, it is still a challenge to control selectivity because of the occurrence of hydrogenation, self-coupling, and hydrogenolysis reactions during the hydrogenation process. It is highly desirable to develop efficient non-noble-metal catalysts for the hydrogenation of nitriles to secondary amines, although several noble metal catalysts have been reported. Herein, we successfully prepared a Cu–Ni/W20O58 catalyst and found that the Cu4.4–Ni0.6/W20O58 catalyst showed a 92.3% yield with initial TOFs of 270.0 h–1 at 373 K and 3 MPa H2 for the hydrogenation of benzonitrile (BN) to dibenzylamine (DBA), which was much superior to that of the monometallic Cu4.4/W20O58 and Ni0.6/W20O58 catalysts. Moreover, the Cu4.4–Ni0.6/W20O58 catalyst could be reused at least 4 times and was effective for the hydrogenation of various nitriles with superior selectivity to secondary amines. Furthermore, the reaction mechanism of BN hydrogenation for the Cu–Ni alloy of Cu4.4–Ni0.6/W20O58 was proposed on the basis of spectroscopic studies such as XRD, TPR, TEM, XAFS, and XPS, kinetic studies such as the effect of BN concentration and H2 pressure, the isotopic effect of hydrogen, and the effect of the reaction temperature and DFT calculations. The rate-determining step was the hydrogenation of benzylidenamine (BI) to the half-hydrogenated intermediate by one H atom over the Cu4.4–Ni0.6/W20O58 catalyst. The Ni–W20O58 interface was responsible for the adsorption and activation of BN, and the electron-rich Cu acted as the site for H2 dissociation; the synergistic effect of Cu and Ni led to the superior catalytic performance of the Cu4.4–Ni0.6/W20O58 catalyst.
研究领域:
催化化学
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材料科学
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环境化学
✓ 已验证
产品关联
DOI
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2021
·Vol. 2021
·期 35
·3601-3610
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IF 2.524
Shaozhong Li,Qing Guo,Jin Li,Yongke Hu,Jiayu Lin
Graphical The mesostructured Cu/AlZnO-9 catalyst with 15 wt % Cu was prepared for the hydrogenation of CO 2 to methanol. The well mesostructure increased the exposed Cu surface area and CO 2 adsorption sites, which accelerated the CO 2 conversion, and the ZnO in catalyst increased the generation of methanol. In addition, the well mesostructure heightened the stability of supported Cu catalyst due to the high dispersion of Cu nanoparticles. In this work, the mesostructured Cu/AlZnO catalysts were prepared for the CO 2 hydrogenation to methanol. Experimental results showed that the weight ratio of Al 2 O 3 and ZnO affected the morphology of the mesoporous AlZnO supports and surface properties of the mesostructured Cu/AlZnO catalysts. The AlZnO-9 (the Al 2 O 3 mass within the AlZnO support was 90 wt%) with loose spongy porous structure and high surface area facilitated the Cu nanoparticle dispersion. Thus, the Cu/AlZnO-9 catalyst showed higher exposed Cu surface area ( S Cu ) and more exposed CO 2 adsorption sites, which accelerated the CO 2 conversion. Meanwhile, the ZnO added into catalysts increased the strength of surface basicity and the surface concentration of Zn species, which promoted the catalytic activity of CO 2 hydrogenation to methanol. In addition, the well mesostructure heightened the stability of supported Cu catalyst due to the high dispersion of Cu nanoparticles.
研究领域:
化学工程
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催化材料
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环境科学
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DOI
高影响因子
Journal of Advanced Ceramics
·
2022
·Vol. 11
·期 3
·427-442
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IF 11.534
Zhang Yu,Han Shuai,Wang Mingyuan,Liu Siwei,Liu Guiwu,Meng Xianfeng,Xu Ziwei,Wang Mingsong,Qiao Guanjun
One-dimensional nanofibers can be transformed into hollow structures with larger specific surface area, which contributes to the enhancement of gas adsorption. We firstly fabricated Cu-doped In 2 O 3 (Cu-In 2 O 3 ) hollow nanofibers by electrospinning and calcination for detecting H 2 S. The experimental results show that the Cu doping concentration besides the operating temperature, gas concentration, and relative humidity can greatly affect the H 2 S sensing performance of the In 2 O 3 -based sensors. In particular, the responses of 6%Cu-In 2 O 3 hollow nanofibers are 350.7 and 4201.5 to 50 and 100 ppm H 2 S at 250 °C, which are over 20 and 140 times higher than those of pristine In 2 O 3 hollow nanofibers, respectively. Moreover, the corresponding sensor exhibits excellent selectivity and good reproducibility towards H 2 S, and the response of 6%Cu-In 2 O 3 is still 1.5 to 1 ppm H 2 S. Finally, the gas sensing mechanism of Cu-In2O3 hollow nanofibers is thoroughly discussed, along with the assistance of first-principles calculations. Both the formation of hollow structure and Cu doping contribute to provide more active sites, and meanwhile a little CuO can form p–n heterojunctions with In 2 O 3 and react with H 2 S, resulting in significant improvement of gas sensing performance. The Cu-In 2 O 3 hollow nanofibers can be tailored for practical application to selectively detect H 2 S at lower concentrations.
研究领域:
材料科学
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纳米技术
·
化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）