JOURNAL OF SOLID STATE CHEMISTRY
·
2023
·
IF 3.3
Zehui Liu,Dianjin Ding,Jinzhao Huang,Jun Tang,Sixuan Zhang,Xiaolong Deng
It's still a challenge to design reasonably efficient catalyst using non-noble metal for the oxygen evolution reaction (OER). In this paper, we use a simple one-step electrodeposition method to load Ce and S co-doped NiFe amorphous alloys onto Cu(OH) 2 nanorod arrays. The excellent oxygen electrocatalytic performance of the catalyst NiFeCeS/Cu(OH) 2 /CuF is attributed to the electronic environments of the active sites of Ni and Fe regulated by heteroatomic sulfur and cerium , which promote the transfer of the oxygen precipitation intermediates to the higher valence states. Meanwhile, the highly conductive substrate accelerates the electron transfer efficiency of the catalyst material, and the loose nanostructure increases the specific surface area , exposing more active sites. NiFeCeS/Cu(OH) 2 /CuF shows outsanding electrocatalytic activity for oxygen evolution with a low overpotential of 227 mV at a current density of 10 mA cm −2 in alkaline medium. Moreover, the nanocomposite catalyst also exhibits rapid reaction kinetics and long-term stability and durability. In this work, an efficient oxygen precipitation catalyst is reported, which indicates that non-precious metal-based electrocatalysts have great potential for application in water electrolysis and provides a basis for the rational design and synthesis of nanorod array catalysts with unique structures.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 39
·18476-18484
·
IF 3.3
Bin Liu,Haoliang Ruan,Chengyi Li,Jie Yao,Bei Wei,Lei Wang,Shurong Ban,Jun Xie
In this work, InCex nanoparticles with different In–Ce ratios were synthesized by a simple co-precipitation method and InCex nanoparticles could be used as a mimic of peroxidase to catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) by H2O2 and produce the typical blue ox TMB. In addition, the prepared InCex nanoparticles showed excellent peroxidase-like catalytic properties compared with pure CeO2 and pure In2O3. InCe0.1 exhibited the best peroxidase-like activity, which was mainly attributed to the indium–cerium synergy, which accelerated the TMB and H2O2 electron transfer rate between them. Based on the above findings, a facile and sensitive H2O2 detection system with a sensitive response range of 10–100 μM and a detection limit of 5 μM for H2O2 was successfully proposed. This work synthesizes nanomaterials with peroxidase-like activity by modifying In2O3 through a simple co-precipitation method and offers new insights into the search for novel peroxidase mimics.
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Small
·
2023
·
IF 13.3
Ya-Xiang Han,Chun-Li Hu,Jiang-Gao Mao
The first examples of thioborate-thiosilicates, namely Ca 2 Ln(BS 3 )(SiS 4 ) (Ln = La, Ce, and Gd), are synthesized by rationally designed high-temperature solid-state reactions. They crystalize in the polar space group P 6 3 mc and feature a novel three-dimensional crystal structure in which the discrete [BS 3 ] 3− and [SiS 4 ] 4− anionic groups are linked by Ca 2+ and Ln 3+ cations occupying the same atomic site. Remarkably, all three compounds show comprehensive properties required as promising infrared nonlinear optical materials, including phase-matchable strong second harmonic generation (SHG) responses at 2.05 µm (1.1–1.2 times that of AgGaS 2 ), high laser-induced damage thresholds (7–10 times that of AgGaS 2 ), wide light transmission range (0.45–11 µm), high thermal stabilities (>800 °C), and large calculated birefringence (0.126–0.149 @1064 nm), which justify the material design strategy of combining [BS 3 ] 3− and [SiS 4 ] 4− active units. Theoretical calculations suggest that their large SHG effects originate mainly from the synergy effects of the LnS 6 , BS 3 , and SiS 4 groups. This work not only broadens the scope of research on metal chalcogenides but also provides a new synthetic route for mixed anionic thioborates.
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NUCLEAR TECHNOLOGY
·
2023
·
IF 1.5
Guanghui Wang,Hui He,Yaorui Li,Meng Zhang,Yang Gao,Caishan Jiao
The contaminated solvent from the Purex process is washed with alkaline detergents such as sodium carbonate, which generates a large amount of secondary wastes. Therefore, hydrazine carbonate as a salt-free reagent deserves to be studied in depth. In this study, the Ce(IV), U(VI), and Zr(IV) metal ions in organic phases containing dibutyl phosphate (HDBP) of 30% tributyl phosphate (TBP)–dodecane were washed with hydrazine carbonate. The effects of the oscillation time (1 to 15 min); temperature (25°C to 85°C); cumulative number of washes (one to four times); mass fraction of hydrazine carbonate (0.1% to 20%); volume ratio of the aqueous phase to the organic phase (0.2 to 5); HDBP concentration (0 to 0.4 M); HNO3 concentration (0.05 to 8 M); and concentration of Ce(IV), U(VI), and Zr(IV) metal ions on the removal percentages of Ce(IV), U(VI), and Zr(IV) metal ions in polluted solvents were studied. The results showed that when the organic phase containing 0.02 M HDBP was washed three times with 5% hydrazine carbonate at 25°C, the removal percentages of the Ce(IV), U(VI), and Zr(IV) ions were 96%, 98%, and 94%, respectively. Meanwhile, the retention concentrations of the three in the organic phase were 35, 28, and 78 mg/L, respectively. The increase of the mass fraction of hydrazine carbonate enhances the removal of the metal ions from the organic phase into the aqueous phase. High acid is not conducive to alkaline washing of metal ions. The increase of HDBP concentration not only promotes extraction but also increases the retention capacity of the organic phase and has the most significant effect on Zr(IV). U(VI) promotes the preferential washing of Zr(IV) while Ce(IV) increases the metal retention concentration of Zr(IV) in the organic phase.
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JOURNAL OF THE ENERGY INSTITUTE
·
2023
·
IF 5.7
Jinchang Liu,Tao Qin,Kuo Li,Xin Chen,Qiuxiang Lu,Jin Deng,Xiaodong Luo,Shenfu Yuan
In this work, the promotion mechanism of Ce as Fe and Ni catalyst promoter for the catalytic reforming of biomass pyrolysis volatiles was investigated. Fe–Ni–Ce/biochar catalysts were prepared and evaluated for their catalytic performance under N 2 and steam atmospheres. The yield of Fe–Ni–Ce/biochar catalyzed syngas (H 2 +CO) increased from 224.36 mL/g to 1299.14 mL/g (800 °C) with the change of N 2 to steam atmosphere. The addition of Ce can introduce a large number of oxygen vacancies to the catalyst, and the increase of oxygen vacancies reduces the reaction barrier of the tar, thus promoting the catalytic activity of the catalyst. In the N 2 atmosphere, the electron transfer of Ce 3+ ⇄ Ce 4+ during catalytic process promotes the production of Fe 2+ to ensure the catalytic activity of the catalyst. In the steam atmosphere, Ni will activate the active sites in a steam atmosphere in water molecules. The activated active sites increase the catalyst activity by cyclic reaction with the oxygen vacancies introduced by Ce, resulting in a higher catalytic capacity of Fe–Ni/biochar than Fe–Ce/biochar. To provide the theoretical basis for the preparation of efficient catalysts based on Fe and Ni.
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ANALYTICA CHIMICA ACTA
·
2020
·
IF 5.977
Yan Liu,Lianying Zhang,Qinge Li,Han Dai,Ting Xiang,Gangyi Yang,Ling Li
In this work, a colorimetric assay for visfatin detection is described. The mixed valence state Ce-MOF (MVCM) modified by platinum nanoparticles (Pt NPs) is used as a novel catalyst. MVCM exhibits excellent intrinsic peroxidase-like catalytic activity due to the spontaneous recycling of the Ce(III)/Ce(IV) system. Pt NPs serve not only as a carrier of the –NH 2 -modified single strand DNA (S1) but also as a synergistic catalyst of MVCM. The capture probe (S2) attached to the streptavidin-modified magnetic beads (Mag-SA) could combine with the aptamer to form the Mag-SA/S2/aptamer complex. When in the presence of the target visfatin, aptamer specifically combines with the visfatin, which induces the release of Mag-SA/S2 from the Mag-SA/S2/aptamer complex. At this time, the [email protected] /S1 complex connects with the released Mag-SA/S2, which quickly catalyzes the 3,3,3′,3′-tetramethylbenzidine (TMB), leading to a color change. Under optimal conditions, the absorbance increases linearly when the concentration ranges from 1 ng mL −1 to 100 ng mL −1 , and the detection limit is as low as 0.11 ng mL −1 . Furthermore, Mag-SA/S2 can be reused at least five times by using the uracil-DNA glycosylase (UDG) and an external magnetic field. The proposed method shows satisfying reproducibility, stability, specificity, and sensitivity, and it was successfully applied to detect visfatin in spiked human serum samples. Thus, it has great potential for clinical research, detection, and catalytic applications.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
JiaYu Chen,Peng Fu,Daofei Lv,Yang Chen,Meiling Fan,Junliang Wu,Amogh Meshram,Bin Mu,Xiang Li,Qibin Xia
A high-performance denitration catalyst based on Mn-Ce mixed-oxide derived from a specific Mn/Ce precursorwas fabricated by solvothermal method. It exhibited outstanding low-temperature activity, which achieved above 90% NO x conversion in the temperature of 150–310 °C. Remarkably, Mn-Ce mixed-oxide demonstrated a much better SO 2 tolerance, in which the NO x conversion increased from 92.6% to 97.8% at 150 °C after introducing 200 ppm SO 2 . The synthesized Mn-Ce mixed-oxide has a porous structure with abundant chemisorbed oxygen spices and exposed active sites. In addition, the increased acidity and redox capacity enhanced the catalytic activity after introducing SO 2 . Meanwhile, the injection of SO 2 separates NH 3 adsorption sites from oxidation agents, inhibiting the unwanted oxidization of ammonia to nitrogen oxides. Furthermore, the reaction pathway on Mn-Ce mixed-oxide proved to be the L-H mechanism based on in situ DRIFTS. Thus, the synthesized Mn-Ce mixed oxide demonstrated an excellent denitration performance and the especially high SO 2 tolerance, showing great potential for low-temperature NH 3 -SCR.
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Catalysts
·
2020
·Vol. 10
·期 11
·1329
·
IF 3.52
Shijie Hao,Yandi Cai,Chuanzhi Sun,Jingfang Sun,Changjin Tang,Lin Dong
Monolithic Mn-Fe-Ce-Al-O catalyst with honeycomb cordierite ceramic as a carrier was reported for the first time for low temperature deNOxapplication. In the reaction of selective catalytic reduction (SCR) of NO with NH3, a NO conversion of above 80% at 100 °C was obtained. Notably, the catalyst also showed excellent resistance against SO2and H2O. About 60% NO conversion was maintained after successive operation in the mixed stream of SO2and H2O for 168 h. The Brunner−Emmet−Teller (BET) measurement, SEM, EDS, thermogravimetric analysis (TG), FT-IR, and XPS results of the used catalysts indicated that certain amounts of ammonium sulfate was formed on the surface of the catalyst. XPS results revealed that partial of Fe2+was oxidized to Fe3+during the reaction process, and Fe2+species have strong redox ability, which can explain the decrease in activity after reaction. In addition, SO2and H2O induced a transformation of Ce from Ce4+to Ce3+on the surface of the catalyst, which increased the amount of chemisorbed oxygen. Owing to these factors, the addition of Ce and Fe species contributes to excellent resistance of the catalyst to SO2and H2O.Keywords:honeycomb catalyst;Mn-Fe-Ce-Al-O;low temperature denitration;water and sulfur resistance
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ACS Catalysis
·
2020
·
IF 12.35
Bangxin Li,Shuai He,Jibiao Li,Xiangling Yue,John T.S. Irvine,Deti Xie,Jiupai Ni,Chengsheng Ni
Employment of identical oxides for the cathode and anode in a symmetrical solid oxide fuel cell (SSOFC) is beneficial for decreasing the fabrication costs of a robust cell. Ce doping on the A site of SrFeO3 increased the structural stability in a reducing atmosphere, but ceria was found to exsolve from the perovskite during the cooling process in the air if the doping level reached 20 atom %. The additional doping of 5 atom % Ru in Sr0.8Ce0.2FeO3 on the Fe site could prevent the ceria segregation in air and induce the surface decomposition under fuel conditions for the formation of nanoscale SrO, CeO2, and Ru0. The SSOFC with Ce/Ru codoped SrFeO3 on a Sr- and Mg-doped LaGaO3 electrolyte showed a small Rp value (0.12 Ω cm2) when H2 and ambient air were used as fuel and oxidant, respectively. The peak power densities of 846 and 310 mW cm–2 were achieved at 800 °C using H2 and C3H8 as fuel, respectively. The excellent coke resistance of the anode could be related to the simultaneous in situ exsolution of CeO2, SrO, and Ru0 nanoparticles.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Girma Sisay,Hairus Abdullah,Dong-Hau Kuo,Worku Lakew,Hardy Shuwanto,Sleshi Fentie
The works on photocatalytic hydrogen production and green chemical conversion have received significant attention due to the current need for clean energy and a secure environment. Herein, Ce and Ga codoped Zn(O,S) has been synthesized with different amounts of Ce using facile precipitation method at a low temperature of 95 °C and characterized by XRD, SEM, HRTEM, XPS, EPR, Raman, DRS, PL, EIS, UV–vis, GC–MS, and photocurrent response measurements. The as-prepared photocatalysts were utilized for hydrogen production and hydrogenation of toxic organic compounds, viz. nitrobenzene (NB) and azobenzene (AB) into a valuable product of aniline. The incorporation of Ce and Ga into Zn(O,S) enhanced the hydrogen evolution and hydrogenation reactions of NB and AB. This notable enhancement was ascribed to the synergistic effects of Ce and Ga dopants to form positively charged defects that trap the photogenerated electron. The trapping mechanism improves the photogenerated charge separation and transfer as confirmed with impedance spectroscopy (EIS), transient photocurrent response, and PL measurements. The highest hydrogen production was attained by 15Ce-5Ga-Zn(O,S) with a rate of 7130 μmol∙g − 1 ∙h − 1 in 10% ethanol solution. In addition, NB and AB were effectively converted to aniline in 15 min and 30 min, respectively. A plausible photocatalytic hydrogenation mechanism for both hydrogenation of NB and AB is proposed with the steps of surface adsorption, molecular diffusion, pinning at oxygen vacancy sites, and hydrogenation reaction with the help of in situ generated H + coupled with electrons.
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CERAMICS INTERNATIONAL
·
2021
·
IF 4.527
Xinyu Zeng,Yang Li,Jia Dong,Jingli Li,Zhaoyu Yang,Chunlin Song,Gang Liu,Yan Yan
In the current study, a series of CeO 2 -doped ( x = 0.01, 0.015, 0.02, 0.025 mol) ceramic samples were prepared, and the valence of Ce in the perovskite was analyzed in detail, revealing the polarization contribution and effect mechanism of the doped Ce element in the 0.65BaTiO 3 –0.35Sr 0.7 Bi 0.2 TiO 3 ceramic. The phase structure and electrical stored energy performance of the resulting ceramics were also characterized. It was found that adding an appropriate amount of CeO 2 to BaTiO 3 was helpful for improving the relaxor behavior, promoting electric storage, and releasing ceramic materials. Particularly, the electric breakdown strength of the 0.02Ce-doped specimen reached 330 kV/cm, and the corresponding density and efficiency were 2.57 J/cm 3 and 81.30%, respectively. In addition, doping with Ce caused the ceramics to exhibit good stability at frequencies of 1–300 Hz and over a temperature range of 30–150 °C. A high current density ( C D ) and power density ( P D ) were obtained in charge–discharge tests.
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BIOMATERIALS
·
2019
·
IF 10.273
Zhengwei Liu,Faming Wang,Jinsong Ren,Xiaogang Qu
Notorious bacterial biofilms are becoming severe threats to public health worldwide. As the important component in biofilm extracellular polymeric substances (EPS), extracellular DNA (eDNA) has been manifested to connect different EPS components and bacteria together, leading biofilms hard to eliminate. Herein a series of MOF/Ce-based nanozymes with deoxyribonuclease (DNase) and peroxidase mimetic activities have been designed and synthesized for combating biofilms. The cerium (IV) complexes (DNase mimics) are capable of hydrolyzing eDNA and disrupting established biofilms, while the MOF with peroxidase-like activity can kill bacteria exposed in dispersed biofilms in the presence of H 2 O 2 . This can avoid the recolonization of bacteria and recurrence of biofilms. Given the fact that single-modal antibacterial agent is difficult to drastically eradicate biofilms, the marriage of two kinds of nanozymes is a rational strategy to acquire enhanced performance in combating biofilms. Besides, the utilization of nanozymes circumvents drawbacks of natural enzymes which are costly and vulnerable. Further studies have demonstrated that this kind of artificial enzyme with dual enzyme-mimetic activities can penetrate the biofilms, and inhibit bacterial biofilm formation intensively. Consistently, in vivo anti -biofilm application in treating subcutaneous abscess exhibits commendable wound healing and admirable bactericidal effect . To the best of our knowledge, it is the first time to devise an integrated nanozyme based on the peroxidase-like activity of MOF to eliminate biofilms and kill bacteria on site. This work may promote the application of MOF in the antibacterial field.
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