Catalysts
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2022
·Vol. 12
·期 5
·534
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IF 4.501
Zhaohui Teng,Shan Huang,Na Li,Qulan Zhou
Rice husk ash (RHA) has potential as a supporter of catalysts. In this research, we studied the activity and SO2tolerance of RHA-based Fe-Cu oxide in the reduction of NO by CO. Characterization methods were employed to study the properties of the catalysts and their SO2tolerance. Activity and SO2resistance were also tested at different temperatures. We recommend two catalysts with SO2resistance ability: Fe0.67Cu0.33/RHA (the highest catalytic activity) and Fe0.8Cu0.2/RHA. The NO removal rate hardly changed with the addition of SO2and was kept at about 100%. However, the CO conversion rate decreased with increasing SO2at the lower reaction temperatures, which may be due to the formation of sulfites. Fortunately, the deactivation was reversible and can be reduced with an increase in the reaction temperature. The results of our research may help promote the application of CO-SCR.Keywords:rice husk ash;Fe-Cu catalysts;NO reduction;SO2resistance;CO-SCR
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Di Li,Zengyong Li,Ren Zou,Ge Shi,Yiming Huang,Wu Yang,Wang Yang,Chuanfu Liu,Xinwen Peng
Developing efficient bifunctional electrocatalyst for overall water splitting and conversion of biomass into value-added products at large current density is essential but challenging. Herein, a hierarchical Fe-doped Ni 2 P nanosheets hybridized with C on Ni foam (Fe-Ni 2 P@C/NF) was developed as a robust bifunctional catalyst with excellent catalytic activity for hydrogen evolution reaction (HER) with overpotentials of 75 and 313 mV at 10 and 1000 mA cm −2 , respectively, and as well as for OER with a lower overpotential of 269 mV at 400 mA cm −2 . Particularly, the integrated double-electrode electrolyzer for simultaneous HER and biomass-derived monosaccharide oxidation reaction (MOR) using Fe-Ni 2 P@C/NF only requires a low voltage of 1.55 V to drive a current density of 100 mA cm −2 . Meanwhile, the value-added lactic acid is obtained at the anode. This strategy of coupling biomass oxidation to promote H 2 production can significantly reduce energy consumption and obtain additional high value-added products.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Zongtang Liu,Haini Yang,Mian Wang,Yufeng Sun,Zhenghao Fei,Shujuan Chen,Rui Luo,Lin Hu,Chenggang Gu
Effective removal of polybrominated diphenyl ethers (PBDEs) from the environment is essential for the ecosystem and human health. Reductive debromination of PBDEs by nanoscale zerovalent iron (nZVI) has become an important technology. However, the agglomeration and low persistence catalytic activity of nZVI particles have become urgent problems to be improved. Herein, we report the first application of a new organo-attapulgite (OA) supported Fe/Pd nanoparticles (OA-Fe/Pd) composite for decabromodiphenyl ether (BDE209) removal. BDE209 was efficiently removed using OA-Fe/Pd with a reaction rate that was 9.97 times greater than that of the nZVI due to the synergetic effect of support material OA and Pd loading. OA could prevent nZVI particles from agglomeration and adsorb BDE209 molecules to its surface. Pd could supply atomic hydrogen and also prevent the oxidation of nZVI particles. The degradation of BDE209 by OA-Fe/Pd was affected by many factors and followed pseudo first-order kinetics. The degradation of BDE209 by OA-Fe/Pd underwent a stepwise debromination manner with the H-transfer dominant mechanism. BDE209 (25 mg∙L -1 ) could be degraded to penta-BDEs to diphenyl ether (DE) by 3.0 g∙L -1 OA-Fe/Pd within 240 min under neutral condition. This study provides some inspiration for improving the removal efficiency of PBDEs with nZVI-based materials.
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Small
·
2022
·Vol. 18
·期 9
·2104941
·
IF 15.153
Lixue Yang,Haoqi Yang,Shengyan Yin,Xiuyan Wang,Mingwei Xu,Guolong Lu,Zhenning Liu,Hang Sun
The Fenton-like reaction has great potential in water treatment. Herein, an efficient and reusable catalytic system is developed based on atomically dispersed Fe catalyst by anchoring Fe atoms on nitrogen-doped porous carbon (Fe SA/NPCs). The catalyst of Fe SA/NPCs exhibits enhanced performance in activating peroxymonosulfate (PMS) for organic pollutant degradation and bacterial inactivation. The Fe SA/NPCs + PMS system demonstrates a high turnover frequency of 39.31 min −1 in Rhodamine B (RhB) degradation as well as a strong bactericidal activity that can completely sterilize an Escherichia coli culture within 5 min. Meanwhile, the degradation activity of RhB by Fe SA/NPCs is improved up to 28 to 371-fold in comparison with the controls. Complete degradation of RhB can be achieved in 30 s by the Fe SA/NPCs + PMS system, demonstrating an efficiency much higher than most traditional Fenton-like processes. Experiments with different radical scavengers and density functional theory calculations have revealed that singlet oxygen ( 1 O 2 ) generated on the N-coordinated single Fe atom (Fe-N 4 ) sites is the key reactive species for the effective and rapid pollutant degradation and bacterial inactivation. This work innovatively affords a promising single-Fe-atom catalyst/PMS system for applying Fenton-like reactions in water treatment.
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ANALYST
·
2022
·Vol. 147
·期 5
·956-964
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IF 5.227
Yiyin Zhang,Xiang Gao,Yingwang Ye,Yizhong Shen
Rapid and accurate monitoring of food freshness to provide consumers with high-quality meat continues to be of tremendous importance to the food industry. In this report, an efficient Fe-doped polydopamine (Fe-PDA) nanozyme with peroxidase-mimicking activity was synthesized by a high-temperature hydrothermal method, and was applied to a spectrophotometric sensing system, which successfully reports the concentration of hypoxanthine (Hx) related to meat freshness. The Fe-PDA nanozyme showed excellent peroxidase simulation activity, which was primarily verified by steady-state kinetics experiments. In the presence of xanthine oxidase (XOD), Hx can react quantitatively with dissolved O2 to generate H2O2, which can be further catalyzed and produce hydroxyl radicals (•OH) under acidic conditions via the Fe-PDA nanozyme and oxidize colorless TMB to blue oxTMB with absorbance at 653 nm. The absorbance at 653 nm expressed a clear linear relationship with hypoxanthine concentration in the range of 5.13–200 μM, and the detection limit was 1.54 μM. This method was further assessed by measuring the recovery of Hx added to meat samples, which showed promising accuracy. Overall, the developed Fe-PDA nanozyme with excellent peroxidase-mimicking activity is cost-effective, high-performance and easy to produce, offering an efficient and low-cost sensing system based on spectrophotometry for meat freshness determination as an alternative to conventional methods.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Shuai Liu,Mengmeng Jin,Jiaqiang Sun,Yongji Qin,Sanshuang Gao,Yu Chen,Shusheng Zhang,Jun Luo,Xijun Liu
Electrocatalytic CO 2 reduction reaction (CRR), powered by renewable energy sources, is a promising route to address energy and environmental issues. Herein, we fabricate single atomic Fe sites anchored on B and N co-doped carbon (Fe-SA/BNC), which showed excellent CRR activity, achieving a highest Faradaic efficiency of ∼ 94% at −0.7 V versus reversible hydrogen electrode. The performance is much better than that of the B-free sample. Furthermore, an outstanding current density of ∼ 130 mA cm −2 , as well as ∼ 99% Faradaic efficiency, has been achieved using the membrane electrode assembly (MEA). Details of density functional theory (DFT) calculations revealed that the introduction of B was beneficial for the desorption of *CO. The Zn-CO 2 battery was then assembled, which reached a high peak power density of 1.18 mW cm −2 at a current density of 4 mA cm −2 , as well as showing remarkable stability for CO production.
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APPLIED SURFACE SCIENCE
·
2021
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IF 6.707
Li Li,Zhi Huang,Yanying Liu,Ziqi Zhu,Mingjun Xu,Wenxuan Wei,Qian Zhang,Junming Hong
Novel porous Mn-Fe nanocubes (p-MnFe NCs) with abundant oxygen vacancies, which derived from Mn-Fe prussian blue analogue, were fabricated for the first time through annealing at H 2 atmosphere. Among the different molar ratios of Mn/Fe, p-Mn 1 Fe 1 NCs possessed abundant oxygen vacancies and exhibited excellent performance for peroxymonosulfate (PMS) activation to effectively degrade bisphenol A (BPA). As a result, 100% BPA (20 mg/L) degradation efficiency can be achieved within 30 min in the p-Mn 1 Fe 1 NCs/PMS system. SO 4 •− , HO•, O 2 •− and 1 O 2 were confirmed as main reactive oxygen species during catalytic reaction. The exposed Mn and Fe sites on the surface of p-Mn 1 Fe 1 NCs were the main active sites for the generation of reactive radicals. For non-radical generation pathway, the generated 1 O 2 and O 2 •− mainly originated from the reaction between dissolved oxygen and surface oxygen vacancies, and parts of 1 O 2 originated from the formation of intermediate O 2 •− . Radical and non-radical pathways were proposed in the p-Mn 1 Fe 1 NCs/PMS system for insights into the mechanisms of BPA degradation. Finally, the possible degradation pathways were proposed via ultra-performance liquid chromatography quadrupole time-of-flight mass spectrometry (UPLC-TOF-Q-MS) analysis.
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ACS Sustainable Chemistry & Engineering
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2023
·
IF 8.4
Xinna Zhao,Guangbing Liang,Hui Wang,Zhenping Qu
Platinum (Pt) is a nonrenewable mineral with limited reserves and a patchy distribution. Pt demand and consumption are growing year after year. As a result, recovering Pt from the secondary resources is critical. A new strategy for effective Pt recovery employing Fe(III)-oxalate complexes under UV and visible light irradiation is proposed in this paper. This approach can recover 98.9% of Pt in 30 min under the conditions of 365 nm UV irradiation, leaching time = 30 min, C2O42– concentration = 333.33 g/L, and H2O2 addition = 0.60 vol %. More importantly, 95.6% of Pt can also be recovered in 8 h under sunlight. The homogeneous photocatalytic reaction is rapid and efficient, and meanwhile, no strong acid, base, or volatile toxic organic solvent is required. Additionally, the iron utilized in the process may be well-recycled, solving the problem of recovery difficulty of homogeneous photocatalysts and lowering the cost of leaching. Simultaneously, the Pt complex recovered from the waste catalyst is utilized in situ to manufacture 0.1 wt % Pt/ZSM-5 catalyst, which shows the complete conversion of toluene at 200 °C and can remain stable during the long duration reaction of 1200 min. Overall, it can not only provide a new environmentally friendly technique to recycle Pt from spent catalysts but also save manufacturing cost of new catalysts.
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Journal of Chemistry
·
2023
·
IF 3
Hao Fu,Aotian Gu,Peng Wang,Chunhui Gong,Zhiying Li,Kai Chen,Yi Yang
The exploration of transforming various metals as metal sources into metal organic frameworks (MOFs) has attracted considerable attention in recent years. This study used triethylamine and 5,6-dimethylbenzimidazole (DMBIM) to modify the iron-doped cobalt zeolite imidazole framework on carbon fiber structure. The results showed that the ZIF(Fe/Co)1.25@CNF exhibited high CEF removal efficiency that over 97% of ceftiofur sodium (CEF) was removed within 10 min, which was significantly higher than that of the common ZIF-67 materials. Compared with other ZIF-67 composites, ZIF(Fe/Co)x@CNF has a larger specific surface area, resulting in a larger contact area and more active sites during the reaction. After the introduction of DMBIM, the ZIF(Fe/Co)1.25@CNF not only easily separated from the solution but also enhanced the hydrophobicity, which provided higher catalytic stability and catalytic performance. In addition, the effects of different catalyst ratios, pollutant concentrations, solution pH, and different radicals (•OH, SO4•−, 1O2) on the activation of peroxymonosulfate (PMS) were investigated. The mechanism of degradation was elucidated by electron paramagnetic resonance experiments. This study provides a new perspective for the preparation of high-performance MOF catalysts with excellent catalytic performance and may facilitate the application of MOF materials in more practical situations.
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CHINESE JOURNAL OF CATALYSIS
·
2023
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IF 16.5
Wenqian Yang,Ziqian Xue,Jun Yang,Jiahui Xian,Qinglin Liu,Yanan Fan,Kai Zheng,Peiqin Liao,Hui Su,Qinghua Liu,Guangqin Li,Cheng-Yong Su
The selective electrochemical reduction of CO 2 to CO is a promising solution for the design of carbon-neutral, sustainable processes. Achieving a highly selective single reduction product is still challenging because of the energetically favorable competing hydrogen evolution reaction. We report the fabrication of N-doped sponge-like porous graphitic carbon structures embedded with Fe nanoparticles (Fe@NPC) via the pre-modification of a metal-organic framework (IRMOF-3(Zn)) with carboxyferrocene, followed by pyrolysis . The as-prepared Fe@NPC exhibited a 96.4% CO Faradaic efficiency at –0.5 V RHE and good stability. The exceptional CO 2 reduction performance is attributed to the unique structure of the composite catalyst, which provides abundant hierarchical pores that increase CO 2 adsorption and mass transfer, and active Fe sites that synergistically accelerate the kinetics of CO generation. The in situ attenuated total reflectance-Fourier transform infrared analysis provided proof of the improved ability of Fe@NPC to accumulate the crucial intermediate *COOH compared with other pyrolyzed porous carbons. Fe@NPC was used in a Zn-CO 2 battery that delivered a maximum power density of 3.0 mW cm –2 , evidencing its potential for application in energy-converting devices.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Jiayi Luo,Yunqiang Yi,Guangguo Ying,Zhanqiang Fang,Yifeng Zhang
The content of active components in magnetic biochar, especially Fe(II), is closely related to its activation performance. Therefore, improving Fe(II) content in magnetic biochar is an ideal strategy to enhance the activation performance of magnetic biochar. In this study, the potassium-doped magnetic biochar was prepared and employed to activate persulfate for degradation of metronidazole. The degradation efficiency of metronidazole in potassium-doped magnetic biochar/persulfate system was 98.4%, which was 13.1 times higher than that in magnetic biochar/persulfate system. Free radicals quenching experiments and electron spin resonance analyses confirmed that surface-bound free radicals were responsible for metronidazole degradation followed the order of 1 O 2 > ·OH > SO 4 · - > O 2 · − . The doping of magnetic biochar with potassium increased its Fe(II) content, approximately 3.1 times higher than that of pristine magnetic biochar. The differences in Fe(II) content between potassium-doped magnetic biochar and magnetic biochar were the key reasons for the activation performance differences. Based on the ultra-high pressure liquid chromatography-quadrupole tandem time-of-flight mass spectrometer , the primary degradation intermediates of metronidazole were identified, and possible degrading pathways were proposed. Overall, this work provides an effective strategy to improve the activation performance of magnetic biochar.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Ruihui Gan,Yali Wang,Wenjun Ma,Mahmut Dirican,Sa Zhao,Yan Song,Xiangwu Zhang,Chang Ma,Jingli Shi
It is highly desirable to develop high-efficiency non-precious electrocatalysts toward oxygen reduction reaction (ORR). In this work, Fe 2 O 3 -encapsulated and Fe-Nx-containing porous carbon spheres (Fe 2 O 3 /N-MCCS) with unique multi-cage structures and high specific surface area (1360 m 2 g −1 ) are fabricated. The unique porous structure of Fe 2 O 3 /N-MCCS ensures fast transportation of oxygen during ORR. The combined effect of Fe 2 O 3 nanoparticles and Fe-Nx configurations endows Fe 2 O 3 /N-MCCS (E 1/2 = 0.837 V vs. RHE) with superior ORR activity and methanol tolerance to Pt/C. And, Fe 2 O 3 /N-MCCS exhibits better stability than nitrogen-modified carbon. The characterization results of Fe 2 O 3 /N-MCCS after long-term test reveals its excellent structural stability. Impressively, zinc-air battery based on Fe 2 O 3 /N-MCCS showed a peak power density of 132.4 mW cm −2 and a specific capacity of 797 mAh g −1 , respectively.
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