CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Wenyang Fu,Zhongzheng Hu,Yang Zheng,Pei Su,Qizhan Zhang,Yongli Jiao,Minghua Zhou
Compared to traditional haber–bosch process for synthetic ammonia, electrochemical reduction of nitrate to ammonia (ERNA) offers a promising and sustainable technology to generate ammonia at ambient temperature. However, the performance of ERNA is impeded by lacking of sound strategy for designing high-performance electrocatalyst. Here, a Cu based electrode with Cu 2 O/Cu interface was prepared by pulse electrodeposition and electroreduction, achieving the fast rate constant of 0.14 min −1 for reducing nitrate with a high ammonia yield rate of 2.17 mg cm -2 h −1 (faradaic efficiency: 84.36%) and ammonia selectivity of 94.4% at −0.25 V vs. RHE. Particularly, density functional theory (DFT) calculations for the adsorption energy indicated that Cu 2 O/Cu interface alleviated adsorption energy of NO 2 - from −2.02 eV (pure Cu) to −1.59 eV, improving surface diffusion of adsorbed NO 2 - . And DFT calculations for electronic structure implied that Cu 2 O/Cu interface upshifted the d band center of Cu (-2.25 eV vs. −2.48 eV of pure Cu), boosting electron transfer to NO 3 - . Additionally, in-situ infrared spectroscopic analysis confirmed vital intermediates of NO 2 - and NH 2 OH on Cu 2 O/Cu to identify reaction pathway and Gibbs free energy diagram clarified this interface decreased reaction barrier of crucial step (reducing *NO 2 to *NO) from 0.31 eV (pure Cu) to −0.77 eV for the enhancement of ERNA. Thereby, these findings demonstrated that Cu 2 O/Cu interface tunes mobility of NO 2 - and electron transfer to NO 3 - on Cu based electrocatalyst is an efficient method to promote performance of ERNA with high efficiency and rate.
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Journal of Materials Research and Technology-JMR&T
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2021
·
IF 5.039
Yuyu Liu,Zheng Chen,Xiaoqin Yang,Jinyong Zhang,Zhonggang Sun,Yuzeng Chen,Feng Liu
Different from the reported catalysts such as metallic glasses ribbons and ball-milled high entropy alloy powder, high entropy alloy nanoparticles (HEA NPs) have attracted wide attention for compelling and functional catalytic properties to degrade methylene blue (MB) dye. CoCrXFeNi (X = Al, Cu, Mn) HEA NPs with different loadings were synthesized by impregnation-adsorption method on activated carbon (AC). Nanoscale HEA NPs with maximized configuration mixing entropy are composed of a single solid-solution face-centered cubic (FCC) phase and the nanocomposites show distinctive porous architectures and large specific surface area (average S BET = 632.7 m 2 /g) for 10 wt.% loadings. The reaction rates ( k o b s ) of 10 wt.% CoCrAlFeNi and CoCrMnFeNi HEA NPs-AC for MB degradation are 0.1998 and 0.1830 min −1 and show comparable intrinsic catalytic performance to amorphous ribbons and HEA powders. The HEA NPs can effectively decompose MB molecule via nanoscale galvanic cell effect which provides a promising material in dye decomposition and mineralization.
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TALANTA
·
2021
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IF 6.057
Hui Huang,Meini Li,Mingwei Hao,Liangli (Lucy) Yu,Yongxin Li
A selective and sensitive colorimetric strategy for sulfide analysis was developed using GMP-Cu nanozymes with a laccase-like activity. This research discovered for the first time that sulfide could significantly enhance the catalytic activity of the GMP-Cu nanozymes by about 3.5 folds. The enhanced laccase activities duo to two reasons. First, Cu 2+ in GMP-Cu nanozymes was reduced to Cu + . The other reason was the formation of Cu–S bond which was beneficial to accelerate the electron transfer rate to improve catalytic activity. Therefore, this method showed an excellent selectivity for sulfide. And it had a linear relationship in the sulfide concentration range of 0–220 μmol/L with a detection limit of 0.67 μmol/L. Furthermore, the proposed method was successfully applied to examine sulfide in the food systems. This new method may be used in sulfide detection to improve food quality and safety.
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PubMed
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Reaction Kinetics Mechanisms and Catalysis
·
2021
·Vol. 133
·期 1
·55-71
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IF 2.081
Yu Jun,Liang Jiezhen,Chen Xiaopeng,Wang Linlin,Wei Xiaojie,Qin Yanmin,Li Youqi,Ling Youkang
The reaction pathway and kinetics of cellulose hydrogenolysis to ethylene glycol (EG) catalyzed by nickel and tungsten combined with copper supported on magnesium aluminum spinel (NiO x -WO y -Cu/MgAl 2 O 4 ) were studied. Cellulose was hydrolyzed to glucose, which followed either the retro-aldol condensation to glycolaldehyde and erythrose or isomerized to fructose followed by retro-aldol reaction to dihydroxyacetone and glyceraldehydes. The derived glucose can also be hydrogenated to sorbitol. The intermediate products were subsequently converted to EG, erythritol, glycerol and 1,2-propanediol. The cellulose conversion, yields of EG and C 2,3 polyols were achieved 100, 53.1 and 62.7%, respectively. The simplified kinetic models were proposed and validated with the experimental results, indicating that the simpler first-order model could perfectly describe the hydrogenolysis of cellulose in the catalytic system. Hydrolysis of cellulose was demonstrated as the rate determining step independent of the reaction pathway, and high temperatures were favorable to the hydrolysis of cellulose to glucose. Activation energies results showed that high temperatures were favorable to the hydrolysis of cellulose to glucose.
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RSC Advances
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2020
·Vol. 10
·期 58
·35374-35380
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IF 3.119
Baozhu Zhang,Chunying Wei
A highly sensitive thrombin aptasensor was constructed based on the alteration of the aptamer conformation induced by the target recognition and the turn-on fluorescence due to the proximity of two darkish DNA-templated copper/silver nanoclusters (DNA-Cu/Ag NCs). Two DNA templates were designed as the functional structures consisting of the Cu/Ag NC-nucleation segment located at two termini or one terminus and the aptamer segment in the middle of a DNA template. Two darkish DNA-Cu/Ag NCs came close to each other when the aptamer combined with the target due to the conformational alteration of the aptamer structure, resulting in an increased fluorescence signal readout. Thrombin was sensitively determined as low as 1.6 nM in the range of 1.6–8.0 nM with a high selectivity. Finally, this sensor succeeded in detecting thrombin in a real fetal bovine serum.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2020
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IF 5.162
Xia-Xiao Wu,Yu Zhang,Tian Hu,Wei-Xiong Li,Zeng-Lin Li,Han-Jian Hu,Shui-Rong Zhu,Wen-Zhao Chen,Chu-Song Zhou,Gang-Biao Jiang
Bone related-bacterial diseases including wound infections and osteomyelitis (OM) remain a serious problem accompanied with amputation in most severe cases. In this work, we report an exceptional effective antibacterial alginate aerogel, which consists of tigecycline (TGC) and octahedral Cu crystal as an organo-inorganic synergy platform for antibacterial and local infection therapy applications. The alginate aerogel could greatly prolong the release of copper ions and maintain effective antibacterial concentration over 18 days. The result of in-vitro experiments demonstrated that the alginate aerogel has an exceptional effective function on antibacterial activity . Cytotoxicity tests indicated that the alginate aerogel has low biological toxicity (average cell viability >75%). These remarkable results suggested that the alginate aerogel exhibits great potential for the treatment of OM, and has a prosperous future of application in bone tissue engineering.
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CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Xue-Qi Zhang,Rong-Fang Shen,Xiao-Jing Guo,Xi Yan,Yan Chen,Jiang-Tao Hu,Wan-zhong Lang
Herein, a convenient and environment-friendly grafting and reduction strategy was used to anchor bimetallic Ag-Cu nanoparticles on polypropylene (PP) fabrics. The as-prepared samples were characterized by various techniques including FE-SEM, XRD, EDX, XPS and FT-IR. The as-prepared sample exhibits excellent activity on the catalytic reduction of highly concentrated 4-NP, and the synergistic effect between Ag and Cu nanoparticles was proved. The entire catalytic reduction was generally considered to obey pseudo-order kinetics, affording high conversion even after 15 successive recycles. These results showed that the PP based composite with Ag-Cu nanoparticles effectively provided superb catalytic efficiency and stability in 4-nitrophenol reduction, and the PP based composites were suitable in practical applications for the treatment of diverse waste water.
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NANOTECHNOLOGY
·
2020
·Vol. 32
·期 8
·085101
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IF 3.551
Yang Sheng,Shuai Li,Yixin Sun,Rong Zhang,Xinyu Zhao,Mei Chee Tan
CuInSe2 quantum dots (QDs) are one of the most important Cd-free fluorescent probes; they usually exhibited low fluorescence intensity, suggesting that a considerable amount of absorbed photon energy was lost as heat. In this study we aimed to improve the fluorescence intensity of CuInSe2 QDs and investigate their photoacoustic (PA) signal resulting from the heat dissipation, which was previously rarely reported. Cu–In–Zn–Se/ZnSe QDs were synthesized by adopting two strategies of Zn doping and ZnSe shell growth. It was found that there was an upper limit for Zn concentration beyond which the fluorescence intensity began to decrease. In addition, a blue shift of the emission peak of Cu–In–Zn–Se/ZnSe QDs was observed at high concentrations of ZnSe precursor due to the diffusion of excessive Zn. To prepare the dual-modal fluorescence and PA imaging probe, poly(maleic anhydride-alt-1-octadecene) (PMAO) modified with polyethylene glycol (PEG) was coated on the QDs, which led to a slight reduction in fluorescence. Cellular labeling on HeLa cells was performed to demonstrate the utility of these probes for fluorescence imaging. We further studied the in vitro PA imaging capabilities of the Cu–In–Zn–Se/ZnSe/PMAO-g-PEG nanoparticles, which showed a distinct PA signal beyond 1.0 mg ml−1. The current work demonstrated that a moderate amount of Zn doping is necessary for enhancing fluorescence and there is a limit beyond which the fluorescence will be diminished. We also demonstrated the proof of concept that Cu–In–Zn–Se/ZnSe QDs are able to serve as a potential PA imaging contrast agent.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
·
IF 4.939
Chongqi Chen,Hongju Ren,Jianke Zhou,Yu Luo,Yingying Zhan,Chaktong Au,Xingyi Lin,Lilong Jiang
Two precursors, namely, p -CFO- T (tetragonal) and p -CFO- C (cubic), were fabricated by a sol-gel method via citric acid and poly(vinyl alcohol) complexation, respectively. After H 2 -reduction, the two were converted to Cu/Fe 3 O 4 catalysts of different complexions, which are named as CFO-CA and CFO-PVA, respectively. The distribution of Fe 2+ and Fe 3+ in the Cu/Fe 3 O 4 catalysts was studied by Raman and XPS techniques. It was disclosed that the distribution of Fe 2+ and Fe 3+ in Fe 3 O 4 has an effect on Cu–Fe 3 O 4 interaction and catalyst surface basicity . Compared to CFO-PVA, CFO-CA has a larger amount of Fe 3+ , which mostly sits at the octahedral sites, leading to stronger Cu–Fe 3 O 4 interaction, and a larger amount of catalyst surface sites that are of weak basicity. As a result, the critical elementary steps of WGS reaction , viz. water dissociation, –COOH decomposition and CO 2 desorption are promoted as reflected in the lower E a and higher catalytic activity of CFO-CA.
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Inorganic Chemistry Frontiers
·
2020
·Vol. 7
·期 17
·3204-3216
·
IF 5.958
Chaoyue Zhao,Xianming Zhang,Ziting He,Qingxin Guan,Wei Li
For acetylene hydrochlorination, as a substitute for toxic mercury catalysts, Cu-based catalysts are probably the most promising and highly active non-noble metal catalysts. Here, density functional theory (DFT) was used to reveal the mechanism for how the NMP ligand significantly promotes the activity and stability of the Cu-catalyzed acetylene hydrochlorination reaction. According to the experimental and DFT results, the high activity of the NMP coordinated Cu-based catalyst is attributed to the catalyst–ligand and substrate–ligand interactions, which stabilize the substrate-Cu(II)-ligand complex in the catalytic cycle. Moreover, the most important two stages were investigated in detail: the reduction of (i) Cuα+ to Cu0 and (ii) Cu2+ to Cu+ during the reaction process. The results demonstrate that the NMP ligand prevents high valence Cu2+ from being reduced due to the geometric distortion influence and the hydrogen bond interaction between the catalysts and ligands. Also, NMP could inhibit the carbon deposition by avoiding the formation of Cu(0) and its strong adsorption of acetylene on the surface.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2020
·
IF 6.551
Dan Wang,Haijun Zhang,Yun Fan,Rong Cao,Yuan Gao,Jiping Chen
The direct chlorination of dibenzo- p -dioxin (DD) and dibenzofuran (DF) is an important source of dioxins in combustion flue gas . The chlorination reaction mainly occurs via electrophilic substitution induced by Cu and Fe chlorides, which must cohabit on particulate matters in mixed state. To explore the mechanism for DD/DF chlorination in real combustions flue gas, 8 kinds of CuO/Fe 2 O 3 /CuCl 2 /FeCl 3 composites impregnated onto silica powder were prepared to simulate the coexisting state of Cu and Fe species in combustion flue gas. Mixed Cu and Fe oxides and chlorides induced a significant synergistic effect on electrophilic chlorination of DD/DF. The efficiencies of DD/DF chlorination over composites containing both Cu and Fe species were 1–2 orders of magnitude higher than those over composites containing only Fe species at 250 °C. CuCl 2 species were highly active sites for electrophilic chlorination. FeCl 3 acted as an excellent promoter to accelerate DD/DF chlorination over CuCl 2 species. The elevated proportion of Cu and Fe oxides was also favora ble for electrophilic chlorination. Compared with DF, DD was more prone to be chlorinated. Chlorine substitution primarily occurred at 2, 3, 7 and 8 positions of DD and DF. Furthermore, the possible mechanism for synergistic effect on electrophilic chlorination of DD/DF was speculated.
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APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Fangke Zhan,Juanjuan Yin,Anqi Zhang,Jingxin Zhou,Mingli Wang,Tifeng Jiao
A seed-mediated co-reduction (SMCR) method that is simple to operate and produces heterogeneous components by the simultaneous co-reduction strategy to grow crystal was used to prepare a bimetallic nanomaterial, composed of two components of uniform metal elements. In this work, three different cationic surfactants were studied to control the morphology of bimetallic compound materials: cetyltrimethylammonium bromide (CTAB), cetyltrimethylammonium chloride (CTAC), and cetylpyridinium bromide (C16Py). Three mature and stable palladium crystal particles and the same number of Pd–Cu bimetallic nanomaterials (BNMs) products were obtained. The system of Pd and Cu bimetallic components, which has a large lattice mismatch, was grown uniformly by atomic layer-by-layer deposition under the SMCR method. The experimental results of BNMs for two nitro compounds (2-NA and 4-NP) were obtained by UV–vis spectral characterization. The prepared BNMs showed excellent catalytic ability in the reduction reaction and completed the catalytic reaction within 93 s. After eight consecutive catalytic cycles, the conversion of the catalytic reaction reached more than 90%. A set of surface-enhanced Raman scattering (SERS) experiments were also used to test the Raman enhancement properties of these BNMs, demonstrating a good SERS enhancement effect and good uniformity. These research results provide a new research topic for the exploration of morphology-controlled bimetal nanomaterials.
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