Nano Research
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2023
·
IF 9.9
Dou Tong,Song Dian,Wang Yiping,Zhao Xuhui,Zhang Fazhi,Lei Xiaodong
Electrocatalytic CO 2 reduction reaction (ECO 2 RR) converts CO 2 to high-value chemical products and promotes the carbon cycle. Sulfur (S)-modified copper (Cu) and bismuth (Bi)-based catalysts have been recognized as promising catalysts for ECO 2 RR. Both of them are highly active for selective formate generation, however, their poor stability and severe competing hydrogen evolution reaction (HER) remain challenging. Herein, S-doped Cu coated with Bi (Bi/Cu-S) is developed to improve ECO 2 RR selectivity to formate. Bi/Cu-S/brass mesh (BM) electrode material for ECO 2 RR was prepared by electrodepositing Bi on the surface of Cu-S/BM nanowires obtained from CuS/BM after the electroreduction. The Faradaic efficiency (FE) of the formate reaches the maximum of 94.3% at −0.9 V vs. reversible hydrogen electrode (RHE) with a partial current density as high as −50.7 mAcm −2 and a yield of 30.7 mmolh −1 cm −2 under 0.5 M KHCO 3 electrolyte. Meanwhile, the FE of formate is higher than 90% in the voltage range of −0.8 to −1.0 V vs. RHE. It also shows good stability at −0.9 V vs. RHE with the FE of formate remaining above 93% after a 10 h reaction. Density functional theory (DFT) calculations demonstrate that the Bi/Cu-S structure promotes the adsorption of CO 2 and effectively inhibits HER by enhancing the adsorption of *H to a great extent, improving the selective conversion of CO 2 to formate. This work deepens the understanding of the mechanism of Cu-Bi-based catalysts and S-modified Cu-based catalysts in selective ECO 2 RR to formate, and also provides a new strategy for catalyst design.
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GREEN CHEMISTRY
·
2023
·
IF 9.8
Tan Li,Jing Su,Linjia Yin,Xiangkun Zhang,Cong Wang,Xinbao Li,Jing Zhang,Kaige Wang
A Cu-based catalyst was developed for one-step solvent-free synthesis of aviation biofuel from biomass-derived ketones, including acetone, cyclopentanone, cyclohexanone, and 2-pentanone. Under the optimal working conditions, the conversion rate of acetone, cyclopentanone, cyclohexanone and 2-pentanone of 100% can be achieved by using Cu/Al2O3. 79.7 c% maximum carbon yield of liquid hydrocarbons with 89.5% selectivity of aviation biofuel was obtained under the conditions of 1.0 MPa H2, 280 °C, and 2 h−1 WHSV. The effects of the calcination temperature on the acidity and basicity of the catalyst, as well as the valence and dispersion of Cu species, were investigated. Based on DFT calculations and in situ DRIFTS results, the preferred adsorption of carbonyl groups and efficient dissociation of hydrogen on Cu+ increased the local concentration of H and feedstock on the catalyst surface, accelerating the rate-determining step that predominated on Cu0. The synergistic effect of Cu0 and Cu+ enhanced the formation of aviation biofuel.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Yu Wang,Fengwen Yan,Jie Wu,Zhijun Huang,Liuting Song,Shunda Yuan
The utilization efficiency of single atoms is limited by the active sites being buried in support. To maximize atom utilization, Cu single atoms are anchored on the external surface of g-C 3 N 4 nanofibers (CNNFs), which are fabricated by partial thermal decomposition and subsequent self-assembly in H 2 O. The abundant N and O-containing functional groups of CNNFs are vital for the loading of Cu. Benefited from the full utilization of Cu sites, CNNF-Cu exhibits excellent Fenton-like catalytic activity for Methylene Blue degradation. The reaction kinetic constant is more than 10 times higher than that of the traditional single-atom catalyst with Cu sites evenly distributed throughout the entire support. CNNF-Cu maintains most of its catalytic activity after five cycle tests, suggesting good stability. This work provides a convenient method to maximize the utilization of single metal atoms for catalytic applications.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Wenli Su,Weizan Guo,Yu Fan
Constructing a bimetallic tandem catalytic system is an effective strategy to promote the CO 2 electroreduction (CO 2 ER) to ethanol. However, it is still difficult to achieve high selectivity for ethanol in the CO 2 ER because most of bimetallic catalysts lack sufficient biphasic boundaries. Herein, a series of novel CuAg bimetallic catalysts (CuAg x @NC) were prepared by anchoring Ag in the Cu-based metal–organic framework (NH 2 -Cu-BDC) followed with high-temperature pyrolysis. The results showed that the Ag in the optimal CuAg 5 @NC catalyst was highly dispersed and anchored on the Cu surface, so the catalyst had sufficient Cu-Ag biphasic boundaries, which resulted in superior C 2 products (especially ethanol) selectivities in the CO 2 ER: the Faradaic efficiency (FE) for ethanol production reached 51.8 % at − 1.0 V, and the FE for total C 2 products reached 82.6 % at − 1.2 V, which were higher than those of most previously reported CuAg electrocatalysts. Analyses of the reaction mechanism showed that the appropriate amount of Ag in the NH 2 -Cu-BDC derivative improved the CO coverage on the catalyst surface, promoted C-C coupling and enhanced the adsorption of key intermediates (such as CH 3 CHO) in the ethanol pathway.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Xiaoxiao Wang,Awei Guo,Yunlong Wang,Zhipeng Chen,Yuxuan Guo,Haijiao Xie,Weilong Shan,Junjie Zhang
Electrochemical conversion of CO 2 into chemical feedstock , such as an energy-dense liquid product (formate), is desirable to address the excessive emission of greenhouse gases and store energy. Cu-based catalysts exhibit great advantages in electrochemical CO 2 reduction reaction (eCO 2 RR) due to their low cost and high abundance, but suffer from low selectivity of formate. In this work, a facile one-pot approach is developed to synthesize CuBr nanoparticle (CuBr NP) that can conduct in situ dynamic restructuring during eCO 2 RR to generate Br-doped Cu NP. The in situ-formed Br-doped Cu NP can afford up to 91.6% Faradaic efficiency (FE) for formate production with a partial current density of 15.1 mA·cm −2 at −0.94 V vs. reversible hydrogen electrode (RHE) in an H-type cell. Moreover, Br-doped Cu NP can deliver excellent long-term stability for up to 25 h. The first-principles density functional theory (DFT) calculations show that the doped Br can regulate the electronic structure of Cu active sites to optimize the adsorption of the HCOO* intermediate, greatly hindering the formation of CO and H 2 . This work provides a strategy for electronic modulation of metal active site and suggests new opportunities in high selectivity for electrocatalytic reduction of CO 2 to formate over Cu-based catalysts.
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LANGMUIR
·
2023
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IF 3.9
Pingtao Ming,Yuanyuan Niu,Yongxin Liu,Jinhao Wang,Haohong Lai,Qing Zhou,Haiyun Zhai
In this study, the synthesis of Cu-MOF-199@multiwalled carbon nanotubes (Cu-MOF-199@MWCNTs) composites was achieved and utilized to create an advanced electrochemical sensor for creatinine (Cre) detection. The composites were modified on a glassy carbon electrode surface through direct drip coating, followed by the deposition of copper nanoparticles (CuNPs) via constant potential deposition. Characterized by various techniques and electrochemical analyses, the Cu-MOF-199@MWCNTs composite increased the CuNPs load, improving the detection sensitivity for Cre. Under optimal conditions, the modified electrode exhibited good linearity across a broad range of Cre concentrations (0.05–40.0 μM) with a low detection limit of 11.3 nM. The developed sensor demonstrated remarkable stability, reproducibility, and selectivity, showing promise in sensitive and accurate Cre detection in serum samples.
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CATALYSIS LETTERS
·
2018
·Vol. 149
·期 1
·77-83
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IF 2.911
Wang Hefang,Fu Qinglong,Zhang Guanyan,Sun Yangyang
Abstract A safe and reductant-free method based on co-reduction of nickel and copper oxides via vacuum thermal treatment has been developed for the synthesis of Ni–Cu alloy nanofibers, which includes electrospinning of a nickel acetate/copper acetate/polyvinylpolypyrrolidone (NiAc/CuAc/PVP) precursor solution, followed by vacuum thermal reduction. On account of the synergistic effect between Cu and Ni, the Ni–Cu alloy nanofibers catalyst with an optimal composition exhibits good catalytic performance for the decomposition of hydrous hydrazine in NaOH solution. Graphical Abstract Ni–Cu alloy nanofibers have been prepared by a vacuum thermal co-reduction method, and further used as catalysts for hydrous hydrazine decomposition.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 34
·23306-23313
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IF 3.3
Guohui Li,Pengyu Li,Zhi Ge,Dawei Yan,Wei Sun,Yuanyuan Sun,Xiaoxia Zhou
Photocatalytic conversion of carbon dioxide into fuels provides an effective approach to realize carbon resource utilization. However, the photocatalytic efficiency is still relatively low due to the recombination of photogenerated charges. Herein, we have designed Cu-doped SnO2 nanoparticles (Cu–SnO2) using a glucose-involved hydrothermal crystallization method for the photocatalytic reduction of CO2. The rich oxygen vacancies facilitated the separation and transfer of photogenerated charges, and the confined effect of the typical mesoporous structure promoted the adsorption of CO2, especially a high density of grain boundaries (GBs) and the doping of atomic Cu would introduce new active sites to activate CO2 molecules. This elaborately designed catalyst exhibited super and stable photocatalytic conversion activity of CO2-into-CO, with a CO optimal yield of 107 µmol g−1 in 4 h, which was 2.75 times that over pure SnO2. In situ Raman results indicated that the CO2 reduction reaction followed a *COOH pathway on Cu–SnO2. This work provides implications for the construction of a catalyst with rich defects in the field of energy and environmental catalysis.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2023
·
IF 3.8
Gaiqin Miao,Lifei Liu,Xia An,Xu Wu
In this work, a high-performance CuNiAl-LDHs catalyst was innovatively synthesized for electrochemical carbon dioxide reduction (CO 2 RR) of methanol (CH 3 OH) through the modulated synthesis of Cu-based layered double hydroxide (LDHs). It was found that the optimal CuNiAl-LDHs has superior CH 3 OH selectivity compared to CuAl-LDHs and CuMgAl-LDHs, with the Faraday efficiency (FE) of 76.4% for CH 3 OH generation at −1.2 V. And their FE and current density (4.8 mA·cm −2 ) remained stable during up to 24 h of electrolysis. Meanwhile, this study confirms the significant performance advantages of CuNiAl-LDHs over their derived composite oxides. Series characterization further proves that the excellent catalytic performance of CuNiAl-LDHs is importantly associated with their richness in Cu + and hydroxyl group (—OH). The research expands the application fields of LDHs compounds. Meanwhile, the series of discoveries provide a new insight for the preparation of CH 3 OH by constructing CO 2 RR.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Yangzhi Xu,Zirui Gao,Yao Xu,Xuetao Qin,Xin Tang,Zhiwei Xie,Jinrong Zhang,Chuqiao Song,Siyu Yao,Wu Zhou,Ding Ma,Lili Lin
Hydrogenation of CO 2 into methanol at low-temperature on Cu-based catalysts is of great significance, but remains challenging to enhance activity. In this paper, we report an inverse catalyst constructed with nano-ZrZnO x supported on Cu particles with outstanding methanol synthesis performance at 220 ℃, two times higher than that of commercial Cu/ZnO/Al 2 O 3 catalysts under the same conditions. Detailed structure characterization and performance evaluation demonstrate that the ZrZnO x mixed oxide serves as the most active oxide-metal interface site for CO 2 hydrogenation. The ZrZnO x /Cu inverse catalyst increases the weak and medium CO 2 adsorption sites which are further demonstrated responsible to the methanol productivity. In situ DRIFTs studies reveal that the inverse interface accelerates the reduction of asymmetric formate intermediates and prevents the generation of CO. The combination of enhanced CO 2 activation capability and accelerated hydrogenation rate of intermediates over the ZrZnO x /Cu inverse catalyst probably contribute to the remarkable methanol synthesis performance from CO 2 .
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Jing Zhu,Hongwei Jiang,Wenwu Wang
The high toxicity and low biodegradability of the phenolic pollutants destroyed the balance of the environment and influenced human health seriously. Here, we developed a three-dimensional coloremetric sensor array for discriminating and determinating phenolic pollutants basing on the distinct Cu/nucleotides MOFs . Firstly, three laccase-mimic Cu/MOFs (Cu/AMP, Cu/CMP, and Cu/GMP) were obtained by regulating the molar ratio of Cu 2+ and nucleotides. Then the Cu/MOFs as the recognition elements of the sensor array catalyzed the pollutants-4-AAP-H 2 O 2 system, obtaining the colored benzoquinone products. Subsequently, the data array obtaining from the combined training matrix (3 Cu/MOFs × 6 pollutants × 5 replicates) was projected into a new dimensional space to obtain the 3D canonical scores, and classified into individual clusters by introducing LDA method. No overlap in their respective LDA plots for the six phenolic pollutants with different concentrations suggested the prominent discriminating performance of the sensor array. Furthermore, the sensor array exhibited high selectivity compared to the “lock-and-key” sensors even other active matrices coexisting in water samples. Importantly, the most influential discrimination factor was used to monitor the levels of the six targets, evidencing the potential application in assessing water pollution and maintaining human health.
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MOLECULES
·
2023
·Vol. 28
·期 15
·5683
·
IF 4.6
Yan Xiao,Nannan Zhan,Jie Li,Yuan Tan,Yunjie Ding
The catalytic upgrading of ethanol into butanol through the Guerbet coupling reaction has received increasing attention recently due to the sufficient supply of bioethanol and the versatile applications of butanol. In this work, four different supported Cu catalysts, i.e., Cu/Al2O3, Cu/NiO, Cu/Ni3AlOx, and Cu/Ni1AlOx(Ni2+/Al3+molar ratios of 3 and 1), were applied to investigate the catalytic performances for ethanol conversion. From the results, Ni-containing catalysts exhibit better reactivity; Al-containing catalysts exhibit better stability; but in terms of ethanol conversion, butanol selectivity, and catalyst stability, a corporative effect between Ni–Al catalytic systems can be clearly observed. Combined characterizations such as XRD, TEM, XPS, H2-TPR, and CO2/NH3-TPD were applied to analyze the properties of different catalysts. Based on the results, Cu species provide the active sites for ethanol dehydrogenation/hydrogenation, and the support derived from Ni–Al–LDH supplies appropriate acid–base sites for the aldol condensation, contributing to the high butanol selectivity. In addition, catalysts with strong reducibility (i.e., Cu/NiO) may be easily deconstructed during catalysis, leading to fast deactivation of the catalysts in the Guerbet coupling process.Keywords:copper catalyst;hydrotalcite;stability;ethanol;butanol
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