Journal of Materials Chemistry C
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2022
·Vol. 10
·期 41
·15656-15663
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IF 8.067
Guangchun Song,Qi Zhang,Shuang Liang,Ying Yao,Menglin Feng,Zainabu Majid,Xiaoyun He,Kunlun Huang,Jin-Cheng Li,Nan Cheng
The rapid, efficient, and low-cost detection of heavy metal ions using sensors has attracted widespread interest from researchers due to the health risks posed by heavy metal pollution. In recent years, single atom nanozymes with uniformly dispersed active centers and precisely designed coordination structures have been developed and used for the rational construction of various sensors. However, there is a lack of technology available to detect heavy metal ions using the catalytic activity of nanozymes. In this study, we investigated the oxidase-like (OXD-like) catalytic activity of the single atom Ce-N-C (SACe-N-C) prepared in our previous studies. Notably, we found that both Fe3+ and Cr6+ could significantly enhance the electron conversion rates of Ce3+ and Ce4+ within the SACe-N-C nanozyme, which contributed to the OXD-like activity of the nanozyme. Therefore, we constructed a time-resolved sensor to detect Fe3+ and Cr6+ using the oxidative activity of the SACe-N-C nanozyme. The LOD for Fe3+ was 34.72 ng mL−1 in the linear range of 0.25–1.5 μg mL−1, and the recoveries were in the range of 88.66–113.24%. The LOD for Cr6+ was 93.65 ng mL−1 in the linear range of 0.5–5 μg mL−1, and the recoveries were in the range of 85.49–111.22%. The sensor could rapidly detect Fe3+ and Cr6+ at 30 s and 60 s, respectively. This study provides a promising time-resolved strategy for the rapid detection of Fe3+ and Cr6+ in food using the OXD-like catalytic properties of the SACe-N-C nanozyme.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Weihua Qin,Mingye Ren,Yuwei Lu,Shaoxia Yang
The two-stage fixed-bed reactor significantly enhanced the phenol degradation efficiency in the heterogeneous Fenton-like reaction. The Cu/Bi-Ce/Al 2 O 3 catalyst, prepared by impregnation-precipitation method, exhibited favorable phenol removal, and the phenol degradation efficiency was ∼32.6 % higher in the two-stage fixed-bed reactor than that in the one-stage fixed-bed reactor under optimal parameters. Moreover, the Cu/Bi-Ce/Al 2 O 3 catalyst had excellent stability in the Fenton-like reaction due to the bismuth doping in the catalyst inhibiting the dissolution of copper ion. The Cu/Bi-Ce/Al 2 O 3 catalyst also displayed efficient purification ability for phenolic municipal sewage in the two-stage fixed-bed reactor. The redox cycles of Cu 2+ /Cu + and Ce 4+ /Ce 3+ were evidenced coexist to enhance the catalyst activity. The quenching experiments demonstrated that the generated singlet oxygen and superoxide anion free radicals dominated the degradation of phenol in the heterogeneous Fenton-like reaction over the Cu/Bi-Ce/Al 2 O 3 catalyst. This study may provide a novel heterogeneous Fenton-like/H 2 O 2 system for degrading organic pollutants in the fixed-bed reactor.
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 21
·8240-8248
·
IF 4.569
Jianfeng Fan,Xiaoqiang Du
Atomic doping and surface engineering are regarded as a promising method for improving their electrochemistry performance toward the water oxidation reaction and urea oxidation reaction (UOR) for layered double hydroxides (LDHs) containing low cost transition metals. However, the mechanism of how foreign ion doping and interface construction enhance catalytic activity remains unclear. In this work, NiFe LDH is reported as an example where Ce (Ce-NiFe LDH) is doped or the interface is constructed with Ce(OH)3(Ce(OH)3@NiFe LDH), and water oxidation and urea oxidation reaction are used as probe reactions. The Ce(OH)3@NiFe LDH material shows superior electrocatalytic performance for the water oxidation reaction (at an overpotential of 220 mV@10 mA cm−2) and urea oxidation reaction (at a potential of 1.40 V@10 mA cm−2), which is one of the best electrocatalytic performances reported so far. After a long time of stability testing, it was found that the catalytic current had significant attenuation, and further characterization showed that the surface of the electrode would be oxidized to oxyhydroxide, which is the true active species. The experimental results demonstrate that foreign Ce and Fe atom doping and interface construction improve the exposure of active centres, enhance the electron transfer rate and reduce the impedance of the NiFe LDH material. It is worth noting that this work provides new ideas for designing efficient, stable and environmentally friendly catalysts for water splitting and urea oxidation by means of doping and interface construction.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Sikpaam Issaka Alhassan,Haiying Wang,Yingjie He,Lvji Yan,Yuxin Jiang,Bichao Wu,Ting Wang,Haiying Gang,Lei Huang,Linfeng Jin,Yongsheng Chen
Bauxite is a widely available Al-O-rich mineral with great potential for abating fluoride. However, low adsorption capacity, a narrow workable pH range, and a lack of clarity on the best removal mechanism hinder its application. In this work, a highly efficient bauxite nanocomposite (Bx-Ce-La@500) was synthesized via doping and pyrolysis , and its fluoride adsorption in industrial wastewater was examined. Doping Ce/La synergistically improved the fluoride adsorption affinity of the composite (from pH PZC 8.0 ~ 10.0) and enhanced the •OH. The materials were characterized by SEM-EDS, BET, XRD, and TGA while XPS, FTIR, and DFT were used to investigate the mechanism of fluoride sorption . Results show that Bx-Ce-La@ 500 has a positive zeta potential of 26.3–23.1 mV from pH 1~ 10. The Langmuir model was the best fit with a maximum adsorption capacity of 88.13 mg/g and removal efficiency up to 100% in 50 ppm F − solution. The high F − removal was attributed to the enhanced surface affinity and the formation of adequate •OH on the material. Except for carbonate and phosphate ions, other ions exhibited negligible effects and the selective removal of F − in real wastewater was high. The main mechanism of adsorption was the ligand/ion exchange and electrostatic attraction.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Kaibang Xiao,Fawen Liang,Jinzhi Liang,Weicheng Xu,Zhang Liu,Biru Chen,Xueding Jiang,Xiaolian Wu,Jianan Xu,Jingzi Beiyuan,Hailong Wang
Bimetallic Fe- and Ce-embedded N-enriched porous biochar (Fe-Ce@N-BC) was synthesized to activate peroxymonosulfate (PMS) for metronidazole (MNZ) removal. 97.5% decay of MNZ was achieved within 60 min in Fe-Ce@N-BC/PMS system. The kinetic reaction rate constant of the Fe-Ce@N-BC/PMS system (0.0566 min −1 ) was 10.5 times higher than that of the BC/PMS system (0.0054 min −1 ). The highly dispersed Fe-Ce oxide nanocrystals serve as PMS activation centers, while the addition of nitrogen source increases the surface area and porosity of biochar, as well as enhances the PMS activation performance. It is noteworthy that graphitic N and C O groups in biochar facilitates the PMS activation via a nonradical pathway and the Fe 2+ /Fe 3+ and Ce 3+ /Ce 4+ participate in the radical pathway. The presence of anion ions of SO 4 2− can promote the MNZ degradation process, while HCO 3 – and Cl − ions suppress the MNZ removal. The MNZ removal using Fe-Ce@N-BC in salty media behavior similarly with that in DDI water, while the decreased removal efficiency in real effluent could be mitigated by prolonging the reaction time. Finally, the degradation intermediate products of MNZ were identified and the pathway was proposed according to LC-MS analysis. The relatively low cytotoxicity of the Fe@Ce/N-BC evaluated by animal cell (A375) and toxicity evolution of MNZ intermediate products strongly suggest huge potential of utilization of the catalyst for aquatic environmental remediation.
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APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Jiasheng Wang,Qingrong Wang,Mengdi Zhao,Ming Bao
Toluene gas-phase oxidation is a green, chlorine-free production process for benzaldehyde but its conversion efficiency is still unsatisfying due to the lack of highly efficient catalyst. Here the selective oxidation of toluene to benzaldehyde over V-Ag-Ce/TiO 2 under an air atmosphere was investigated. The catalyst was prepared by impregnation and characterized by scanning electron microscope (SEM), N 2 adsorption-desorption, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Electron paramagnetic resonance (EPR), H 2 temperature programmed reduction (H 2 -TPR), O 2 temperature programmed desorption (O 2 -TPD), and NH 3 temperature programmed desorption (NH 3 -TPD). The amount of oxygen vacancy and acid of the catalyst can be tuned through adjusting the V:Ag:Ce ratio. Over the optimum catalyst (V:Ag:Ce = 4:2:1, molar ratio), 92% benzaldehyde selectivity with a 27% toluene conversion can be obtained at 550 °C. Medium amounts of oxygen vacancy (0.43) and acidity (0.10 mmol/g) are found to be conducive to the conversion of toluene to benzaldehyde. This study has important theoretical guiding significance for improving conversion efficiency from toluene to benzaldehyde by gas-phase aerobic oxidation.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Zihao Chen,Kai Song,Meiting Guo,Jialin Li,Yan Le,Yu Shen,Fang Wang,Zhongwei Yue,San Ping Jiang
Ce-induced phase separation orchestrates a tri-phase nanocomposite architecture. • Optimized fluorite SDC ratio maximizes the triple-conducting transport network. • Excess pure ion-conducting SDC phase critically impedes charge transfer pathways. • SSCC1 delivers 1.64 and 1.30 W cm −2 in SOFC and PCFC modes at 650 °C. • The optimized cell shows exceptional reversible cycling stability over 240 h. Developing multiphase nanocomposite is an interesting approach for the air electrodes with high activity and durability for both solid oxide fuel cells and protonic ceramic cells. Herein, a Ce-induced phase separation strategy is reported to construct a multiphase nanocomposite (Sm 0.6 Sr 0.4 Co 0.9 Ce 0.1 O 3−δ ) comprising single-perovskite Sm 0.5 Sr 0.5 CoO 3-δ (SP-SSC), Ruddlesden-Popper SrSm 2 Co 2 O 7 (RP-SSC), and fluorite Sm 0.4 Ce 0.6 O 1.8 (SDC) phases. By precisely tailoring the phase proportions to balance proton, oxygen-ion, and electron conducting networks while maximizing active heterointerfaces, the optimized architecture unlocks exceptional oxygen electrocatalytic kinetics. The results reveal that exceeding the optimal ratio of the fluorite phase impedes charge transfer, highlighting the crucial role of delicate phase regulation. Furthermore, Density Functional Theory calculations reveal that this multiphase network enables a phase-specific division of labor, successfully achieving spatial decoupling of O 2 and H 2 O adsorption to mitigate their competitive adsorption. Consequently, the optimized composite electrode achieves remarkable peak power densities of 1.64 W cm −2 in SOFC mode and 1.30 W cm −2 in protonic ceramic fuel cell mode at 650 °C. Furthermore, an outstanding electrolysis current density of −2.19 A cm −2 at 1.3 V is attained, alongside robust reversible cycling stability over 240 h. This work provides significant insights into designing highly efficient multiphase air electrodes intended for future reversible ceramic electrochemical energy conversion.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xueqin Wang,Tiesen Li,Chan Wang,Qingyan Cui,Tinghai Wang,Xiaojun Bao,Yuanyuan Yue
Designing a cost-effective and fast fabrication Cu-SSZ-13 with improved selective catalytic reduction of NO by ammonia (NH 3 -SCR) performance remains an open question. Here we report that LaCe-SSZ-13 zeolites were synthesized from spent fluid catalytic cracking catalyst within 12 h. After ion-exchanging with CuSO 4 solution, the obtained LaCeCu-SSZ-13 catalysts exhibit significantly higher catalytic activity and hydrothermal stability than conventional Cu-SSZ-13. Various characterizations reveal that La and Ce modification not only facilitates the disperse of isolated Cu 2+ species, but also effectively mitigates dealumination and inhibits copper species aggregation after hydrothermal aging. In-situ diffuse reflection infrared Fourier transform spectrum analyses demonstrate that La and Ce modification can accelerate the adsorption capacity for NH 3 and NO x and promote the decomposition of NH 4 NO 3 intermediate species on the catalyst, benefiting the improvement of low-temperature activity. The combination of experiments and theoretical calculations further demonstrate that the most stable positions of La and Ce are on different eight-membered rings in SSZ-13, and then Cu 2+ ions tend to enter eight-membered rings to enhance the NH 3 adsorption capacity and decrease the H 2 O adsorption capacity, which results in higher low-temperature activity and hydrothermal stability than Cu-SSZ-13. Our work provides a feasible strategy for preparing the efficient rare-earth-modified Cu-zeolite based NH 3 -SCR catalyst for nitrogen oxide abatement.
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CHEMOSPHERE
·
2023
·
IF 8.8
Zeyi Wang,Rong Su,Maojie Zhao,Luyao Zhang,Lu Yang,Feng Xiao,Weishan Tang,Lichuan Chen,Ping He,Dingming Yang
The application of PbO 2 for electrochemical oxidation technology is limited by its low electrocatalytic activity and short service life. Herein, based on the facile one-step electrodeposition , we prepared a boron carbide (B 4 C) and cerium (Ce) co-modified Ti/PbO 2 (Ti/PbO 2 –B 4 C–Ce) electrode to overcome these shortcomings. Compared with Ti/PbO 2 electrode, the denser surface is displayed by Ti/PbO 2 –B 4 C–Ce electrode. Meanwhile, electrochemical characterization indicates that the introduction of B 4 C and Ce significantly enhance the electrochemical performance of PbO 2 electrode. In degradation experiments, under optimized conditions (current density 20 mA cm −2 , pH 9, 0.15 M Na 2 SO 4 and 30 °C), the fully degradation of tetracycline (TC) can be completed within 30 min. Furthermore, the trapping experiment demonstrates that ∙OH and SO 4 ·- radicals have a synergistic effect in the degradation process of TC. Based on results of liquid chromatography-mass spectrometer, the generated ·OH preferentially attacks amides, phenols and conjugated double bond groups in TC. Importantly, Ti/PbO 2 –B 4 C–Ce electrode maintains a constant degradation efficiency even after 10 recycling tests, and its service life is 2.4 times of traditional Ti/PbO 2 electrode. Hence, Ti/PbO 2 –B 4 C–Ce electrode is a promising electrode for degradation of organic wastewater containing amides, phenols, and conjugated double bond groups.
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Scientific Reports
·
2021
·Vol. 11
·期 1
·1-13
·
IF 4.38
Tang Xi,Zhang Yifei,Li Weiqi,Geng Jinju,Ren Hongqiang,Xu Ke
Humic acid (HA) is the main component of organic matter in effluent from wastewater treatment. The effective removal of HA is significant. In this study, a novel catalyst was prepared using a transition metal oxide as the active component and Al 2 O 3 as a granular carrier. The mechanism of catalytic ozonation of HA under neutral pH conditions and its efficiency were investigated. Under the chosen conditions (an ozone concentration of 2.2 mg/L, 50 mg/L HA solution, catalyst dosage of 5 g/L and initial pH of 6.49), the Cu/Ce–Al 2 O 3 bimetallic catalyst led to 54.79% TOC removal rate after 30 min; the removal rate by ozone alone was only 20.49%. The characteristics of organic compounds determined by FT-IR and GC–MS showed that organic compounds were degraded significantly by the catalytic treatment. The addition of catalysts could effectively degrade toxic intermediates and reduce the acute toxicity produced by ozonation. Humic acid substances were largely removed and transformed into biodegradable intermediates. This study proposes a new and efficient ozonation catalyst for practical applications in advanced wastewater treatment.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
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2020
·
IF 4.495
Qiang Liu,Yang Wang,Xin-Yuan Hua,Biao Zhang,Hao-Qian Zhang,Jun-Wei Liu,Feng Ye,Wen Wang
Although traditional functionally graded materials (FGMs) have weakened a certain extent abrupt changes along interfaces between layers, eliminating residual abrupt interfaces which results in great inter laminar stresses remains a major challenge. Herein, ceramic scaffolds with novel continuously graded channels have been firstly prepared through combining layer-by-layer casting with gelation-freeze-dry. Followed by infiltrating soft phase, the co-continuous FGMs without delamination and abrupt changes between layers can be successfully fabricated. The wet layering of suspensions and continuous ice crystals across the interface are the main reasons for the eliminated interfaces. More importantly, the performance of FGMs can be optimized to meet the practical requirement attributed to the varied porosity and pore size distribution of freeze-cast ceramic scaffolds. The novel process for co-continuous ceramics/ FGMs without abrupt interfaces can be extended to other polymers or even metals.
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FUEL
·
2020
·
IF 5.578
Liguang Dou,Mingkai Fu,Yuan Gao,Lei Wang,Cunji Yan,Tianzeng Ma,Qiangqiang Zhang,Xin Li
Direct hydrogenation of CO 2 to synthetic natural gas at a lower temperature remains a big challenge especially in the presence of H 2 S impurity. This contribution describes the synthesis, structure, morphology and doping effect of a series of robust catalysts for CO 2 methanation under resistive heating, based on Ni-layered double hydroxides (LDH) grown on porous and electrically conductive nickel foam (NF) derived structured catalysts. As a result, LaNi/NF showed the highest CO 2 conversion (55%) and CH 4 formation rate (631.5 mmol·g −1 ·h −1 ) at lower temperature of 250 °C and FeNi/NF gave the optimal conversion at 350 °C (75%, 860.9 mmol·g −1 ·h −1 ), which was superior to the most of recently reported Ni-based supported catalysts. We found that the CH 4 selectivity of the H 2 S (50 ppm) poisoned catalysts was significantly decreased and CO was verified as the main by-product. In this case, LaNi/NF and FeNi/NF still retained much higher conversion rate at 300 °C, 29.8% for LaNi/NF and 27% for FeNi/NF, than the almost deactivated unmodified Ni/NF with maximum 5% CO 2 conversion. The extraordinary activities can be explained as that the dopants can greatly strengthen the metal-support interaction and further enhance the reducibility of active metallic Ni, as XRD, HRTEM, TPR and XPS indicated. Besides of this, DFT calculations demonstrated that the existence of La can greatly promote CO 2 adsorption by lowering the adsorption barrier from 0.55 eV of pure Ni to 0.12 eV, and further inhibit the gaseous H 2 S from chemisorbing on the catalyst surface owning to the relatively unstable Ni-S bond.
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