RSC Advances
·
2023
·Vol. 13
·期 11
·7614-7620
·
IF 3.9
Lei Wei,Yanhong Lu,Ruixuan Lu,Yuxin Cui
Hydrolytic dehydrogenation of ammonia borane is a significant and promising approach for on-site hydrogen production at ambient conditions, and developing highly efficient and low-cost catalysts has attracted considerable attention. Herein, waste-biomass-derived activated carbon (AC) was prepared by hydrothermal carbonization and alkali-assisted activation, and non-precious bimetal phosphides (Co–Cu–P) nanocatalysts with a series of different Co/Cu ratios were synthesized on the AC surface through in situ phosphidation method. Owing to the synergetic effects, the optimal Co0.8Cu0.2P/AC presents an outstanding turnover frequency of 26.5 min−1 (25 °C), which is much higher than that of many reported catalysts. The reaction activation energy was measured to be 34.6 kJ mol−1. Benefiting from the ferromagnetic nature of the phosphides, the Co0.8Cu0.2P/AC can be magnetically separated and reused again. After recycling six times, the catalyst still retains 72% of the initial activity, thus indicating great potential for practical applications.
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Nano Research
·
2023
·Vol. 16
·期 5
·6670-6678
·
IF 9.9
Jing Tianyun,Yang Shaokang,Feng Yonghai,Li Tingting,Zuo Yunpeng,Rao Dewei
Co-based catalysts are promising alternatives to precious metals for the selective and effective oxidation of 5-hydroxymethylfurfural (HMF) to the higher value-added 2,5-furandicarboxylic acid (FDCA). However, these catalysts still suffer from unsatisfactory activity and poor selectivity. A series of N-doped carbon-supported Co-based dual-metal nanoparticles (NPs) have been designed, among which the Co-Cu 1.4 -CN x exhibits enhanced HMF oxidative activity, achieving FDCA formation rates 4 times higher than that of pristine Co-CN x , with 100% FDCA selectivity. Density functional theory (DFT) calculations evidenced that the increased electron density on Co sites induced by Cu can mediate the positive electronegativity offset to downshift the d-band center of Co-Cu 1.4 -CN x , thus reducing the energy barriers for the conversion of HMF to FDCA. Such findings will support the development of superior non-precious metal catalysts for HMF oxidation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yeshuang Wang,Xuan Liu,Mingxian Duan,Chaonan Zhang,Huiling Fan,Chao Yang,Tingting Jiao,Tian Kou,Ju Shangguan
Isoreticular bimetal M−Cu−BTC has considerable potential in improving the sulfides removal performance of Cu–BTC. Herein, three transition metals, namely, Zn 2+ , Ni 2+ and Co 2+ , were assessed to fabricate M−Cu−BTC, a desirable isoreticular bimetal. Results demonstrated the feasibility of using Zn 2+ to fabricate an isoreticular bimetallic Zn–Cu–BTC. The Zn 2+ doping content of Zn–Cu–BTC was varied to investigate its influence on the hydrogen sulfide (H 2 S) and methyl sulfide (CH 3 SCH 3 ) removal performance of Cu–BTC. The experimental results indicated that the sulfides removal performance of Zn–Cu–BTC increased and then decreased with increasing Zn doping content. The highest H 2 S and CH 3 SCH 3 removal capacities of 84.3 and 93.9 mg S/g, respectively, were obtained when the Zn 2+ doping content was 17%. The hybridisation of Zn and Cu in Zn–Cu–BTC induced a strong interaction between them. This interaction increased the binding energies of H 2 S and CH 3 SCH 3 towards the Cu and Zn adsorption sites while weakening the bond order between Zn and Cu. The weakened bond order made the Zn–Cu bonds easier to form metal sulfides during desulfurization process, thereby synergistically enhancing sulphide removal.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Li Feng,Xiaoyun Lin,Junhui Feng,Xiaoqin Min,Yongnian Ni
This study presents the preparation of a novel electrochemical non-enzymatic sensor for the detection of glucose in natural saliva based on a metal organic framework (MOF) derivative (Cu-MOF-C) and nickel nanoparticle (NiNP) composite modified glassy carbon electrodes (GCE). The morphology and structural evolution were thoroughly characterized using scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), ultraviolet and visible spectrum (UV) and Fourier transform infrared spectrum (FTIR). Moreover, the electrocatalytic activity of the NiNPs/Cu-MOF-C/GCE for glucose was investigated using cyclic voltammetry (CV) and the amperometric i-t technique. The NiNPs/Cu-MOF-C/GCE sensor exhibits a wide linear range of 0.3–1150 μM and low detection limit (DL) of 0.090 μM at a signal/noise ratio (S/N) of 3. The average recovery rate of this method is satisfactory between 97.3% and 108.4%. Furthermore, the sensor exhibited excellent repeatability, good stability and reproducibility for glucose detection. Compared with traditional invasive measurement, the detection of glucose in natural saliva can reduce the pain caused by continuous blood collection, which is an ideal method for patients requiring continuous monitoring of glucose.
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RSC Advances
·
2023
·Vol. 13
·期 13
·8915-8922
·
IF 3.9
Tong Zhou,Haitang Wei,Bin Xiao,Tianping Lv,Liangfei Duan,Qingjie Lu,Jin Zhang,Yumin Zhang,Qingju Liu
One of the most promising strategies for producing hydrogen is photocatalytic water splitting, in which the photocatalyst is a key component. Among many semiconductor photocatalysts, g-C3N4 has attracted great attention due to its narrow band gap, excellent stability and low cost. However, practical application is limited by its poor intrinsic activity. In this work, a high-performance porous g-C3N4 (PCN) photocatalyst with anchored Cu single atoms (CuSAs) was synthesized by a one-step co-heating approach. The obtained Cu1.5–PCN displays an excellent hydrogen evolution rate (HER) of 2142.4 μmol h−1 g−1 under visible light (=420 nm), which is around 15 and 109 times higher than those of PCN and bulk g-C3N4, respectively. In addition, it also shows good stability during H2 evolution. The results of experimental research and DFT simulations indicate that the single Cu ions formed bonds with the N-ring and these remain stable. Meanwhile, the special electronic structure of the Cu–N charge bridge extends the light absorption band to the visible-light region (380–700 nm). This high-performance and low-cost photocatalyst has great potential in solar energy conversion.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 12
·6191-6197
·
IF 11.9
Hongzhou Yang,He Huang,Qing Wang,Lu Shang,Tierui Zhang,Shouguo Wang
3d transition metal single atom catalysts (SACs) (e.g. M = Fe, Co, Cu) are considered as promising catalysts for oxygen reduction reaction (ORR), among which Fe SACs display comparable performance to commercial Pt/C. However, Fe SACs still demand significant improvements in activity and stability for further industrial deployment. Herein, a Fe, Cu dual metal SAC was synthesized using a facile ligand-mediated method. Fe and Cu atoms were atomically dispersed on commercial carbon black in the form of FeN4 and CuN4 sites. Owing to the interactions between the adjacent Fe and Cu atoms co-existing in a very tiny area, the as-synthesized Fe, Cu dual metal SAC exhibited excellent ORR performance with a high half-wave potential of 0.926 V and good stability in 0.1 M KOH, which are significantly higher than that of the Fe-SAC or Cu-SAC control samples. Density function theory calculations showed that the Cu single atom can act as an electron donator enriching the electron density of Fe sites, thus endowing the Fe sites with optimized adsorption/desorption energy for ORR intermediates and thereby facilitating the ORR activity of FeCu-SAC. Moreover, a study on three typical commercial carbon substrates indicated that carbon support with high surface areas and hierarchical pore structure was beneficial for ORR. The excellent ORR activity and durability of FeCu-SAC enabled the constructed Zn–air battery to have a high power density of 201.4 mW cm−2 and high specific energy of 827.68 W h kg−1.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Shiyao Lu,Jian Zhang,Hao Meng,Xiaoyuan Qin,Jianbin Huang,Yehao Liang,Feng-Shou Xiao
The direct dehydrogenation of ethyl lactate (EL) to produce ethyl pyruvate (EP) over non-precious heterogeneous catalysts is highly desirable, but challenging. Herein, we report a highly efficient silica-supported copper catalyst prepared via a hydrolysis-precipitation method (Cu/SiO 2 -HP) for the dehydrogenation of ethyl lactate, which exhibited an 85.4 % EL conversion with 91.1 % selectivity toward EP at 320 °C. XAFS, in situ XPS, and CO-adsorption FT-IR spectra revealed that the Cu/SiO 2 -HP catalyst had abundant Cu 0 /Cu + interfaces. In situ FT-IR spectra, kinetic studies , and theoretical calculations also demonstrated that the Cu 0 /Cu + interfaces synergistically activate the O−H and C−H bonds in the adsorbed EL for direct dehydrogenation into EP. The H/D kinetic isotope effect for model reaction confirmed that C−H bond activation is the key step in the dehydrogenation reaction. This study offers a new approach toward the selective conversion of EL into EP, which is of great significance for biomass conversion .
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CHEMOSPHERE
·
2019
·
IF 5.108
Yufan Chen,Yong Feng,Huaqiang Chu,Deli Wu,Yalei Zhang
Cu(II) enhanced the oxygen activation by Fe(II) to increase the yield of oxidants. However the factors controlling the catalytic performance and indeed the underlying influencing mechanisms remained unclear. Here, we presented the detailed study of Cu(II)-Fe(II) reactions for a range of pH and Cu(II)/Fe(II) ratios. From the results obtained, we provided insight into the factors controlling the redox reactions of Fe-Cu and the catalytic behaviours of active species. A reaction scheme for the Fe(II)/Cu(II) system was developed in which the in-situ formed Cu(I) mainly contributed to producing H 2 O 2 and Fe(II) dominantly decomposed H 2 O 2 to hydroxyl radical (HO ) [see companion article] (Yufan Chen). Circumneutral conditions facilitated the catalytic processes; under acidic conditions, the reverse reaction between Fe(III) and Cu(I) was strongly favoured; alkaline conditions improved the reducing capacity, which subsequently enhanced the generation of Cu(0) instead of Cu(I). There was a saturated Cu(II)/Fe(II) ratio above which further addition of Cu(II) could not be reduced, and then excessive Cu(I) and Cu(II) consumed HO and O 2 – , respectively. Therefore, the highest removal efficiency of organic pollutants was achieved when the stoichiometric Cu(II)/Fe(II) ratio was 60% at circumneutral pH. The new findings have implications for the treatment of mixed wastewater where copper and organic pollutants coexist.
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FREE RADICAL BIOLOGY AND MEDICINE
·
2019
·
IF 5.657
Hong Huang,Xiaobing Lou,Bingwen Hu,Zhongneng Zhou,Jinquan Chen,Yang Tian
In the amyloid plaques , a signature of AD, abnormally high Cu 2+ concentrations are found bound to Aβ. Most of previous studies reported that Cu-Aβ could contribute to oxidative stress , as H 2 O 2 and •OH are catalytically generated by Cu-Aβ with the assistance of biological reductant, with only one recent report stated that free O 2 •- is also generated in the Cu-Aβ catalyzed processes, where an indirect technique was applied. To comprehensively investigate the free radicals produced during this Cu-Aβ-mediated process with a biological reductant, DNA-cleavage assay, an indirect method, and two direct methods including electron paramagnetic resonance (EPR) spectroscopy and transient absorption spectroscopy (TAS), both having qualitative and quantitative power, were employed in this work. All the experimental results obtained from the three methods demonstrated that Cu-Aβ in the biological reducing environment was not only able to catalyze the production of H 2 O 2 and •OH, but also to generate free O 2 •- . The results further indicated that O 2 •- was the precursor of H 2 O 2 and •OH. It is also important to note that the results obtained from EPR spectroscopy and TAS provided direct evidence for the presence of O 2 •- and •OH. By virtue of the direct techniques, we also found that the longest peptide fragments of Aβ 16 , Aβ 40 , and Aβ 42 produced the least radicals with a lowest rate. More interestingly, the fibrillar forms of Aβ generated less O 2 •- and •OH compared with oligomeric and monomeric forms.
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APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Yuewen Lu,Jin Chen,Ruihao Wang,Pengfei Xu,Xingquan Zhang,Bing Gao,Changping Guo,Guangcheng Yang
Simultaneous improvement of the safety performance and thermal decomposition properties of ammonium perchlorate (AP) remains a significant challenge. Therefore, based on inspiration from biological materials, we have prepared a novel copper alginate/ammonium perchlorate (Cu-alginate/AP) composite by facile air atomization. The evaluation of the safety performance and thermal decomposition indicates that these properties were significantly improved. In addition, the possible catalytic mechanism of thermal decomposition of AP is proposed herein. It should be noted that Cu-alginate is a three-dimensional network structure and was uniformly coated on the surface and inside of the AP. When the composite is stimulated by external forces, this unique structure plays a buffering role, absorbing energy and greatly improving safety performance. With increasing temperature, the Cu-alginate easily decomposed and renascent Cu-based nanoparticles were generated by in situ growth. These renascent nanoparticles exhibited excellent catalytic activity for the thermal decomposition of AP. As expected, the bio-inspired material can smartly improve both the safety performance and thermal decomposition of AP. Therefore, these findings provide a promising strategy for the development of composite solid propellants.
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ACS Catalysis
·
2019
·
IF 12.221
Yue Ma,Songqi Cheng,Xiaodong Wu,Yunzhou Shi,Li Cao,Liping Liu,Rui Ran,Zhichun Si,Jianbo Liu,Duan Weng
Solid-state ion-exchange (SSIE) is an effictive method to prepare Cu-SSZ-13, but usually requires high temperatures or assistance of NH3 for catalyst activation. Herein, an environmentally friendly low-temperature solid-state ion-exchange (LT-SSIE) method was developed. Cu salts that can decompose at temperatures lower than 300 °C (e.g., CuAc2 and Cu(NO3)2) were chosen as Cu precursors. An impregnation method was adopted to obtain high dispersion of the precursors inside the channels of SSZ-13, as confirmed by scanning transmission electron microscopy. A calcination in air at 300 °C for 30 min was found enough for catalyst activation. In situ X-ray diffraction, diffuse reflectance infrared Fourier transform spectroscopy, thermogravimetry, ultraviolet–visible spectroscopy and H2 temperature-programmed reduction were performed to monitor the activation prcoess of CuAc2-impregnated SSZ-13. The ion-exchange sites of SSZ-13 are occupied by Cu2+ ions originating from CuAc2 at 250–300 °C, revealing the nature of the LT-SSIE process between CuAc2 and SSZ-13.
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GREEN CHEMISTRY
·
2019
·Vol. 21
·期 3
·606-613
·
IF 9.405
Zhenbing Xie,Bingfeng Chen,Haoran Wu,Mingyang Liu,Huizhen Liu,Jianling Zhang,Guanying Yang,Buxing Han
Transformation of biomass or biomass-based feedstocks into fuels or valuable chemicals is of great importance for the sustainable development of our society. Mesoporous Al2O3–ZrO2 with different Al : Zr molar ratios was prepared by the sol–gel method, and Cu–Ni/Al2O3–ZrO2 catalysts were fabricated by the impregnation method. The catalytic performances of the bifunctional catalysts were studied in the selective hydrogenation of levulinic acid (LA) into 2-methyltetrahydrofuran (MTHF). It was demonstrated that both Cu : Ni and Al : Zr ratios affected the selectivity to MTHF significantly. The bimetallic catalysts Cu–Ni/Al2O3–ZrO2 containing 10 wt% Ni and 10 wt% Cu gave 99.8% MTHF selectivity at full conversion of LA when the Al : Zr ratio was 9 : 1. The outstanding catalytic performance of the catalyst is related to the mesoporous structure, the acidic properties of the support and the synergistic effect between Cu and Ni. The catalyst could be reused five times without a considerable loss of catalytic activity and selectivity.
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