COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Hongyan Tang,Xuebin Wang,Caiyan Wang,Tiantian He,Jincheng Wang
A composite soil conditioner based on Fe-doped hydroxyapatite/polydopamine/amino carbon nanotubes (Fe-HAP@PDA@CNT-NH 2 ) was prepared for controlling release of flavic acid (FA) fertilizers and for the treatment of soil contaminants methylene blue (MB). Firstly, Fe-doped hydroxyapatite (Fe-HAP) was prepared by hydrothermal method. Then, Fe-doped hydroxyapatite/polydopamine/aminocarbon nanotube (Fe-HAP@PDA@CNT-NH 2 ) composite was prepared by in situ polymerization of dopamine (DA) with amino carbon nanotubes (CNT-NH 2 ) on the Fe-HAP surface. Finally, Fe-HAP@PDA@CNT-NH 2 @FA composite soil conditioner was obtained by loading with FA. Scanning electron microscopy (SEM), X-Ray diffraction (XRD) and Fourier transform infrared spectroscopy (FTIR) were applied to analyze the composition and morphology of the composites. The loading and slow release experiments showed that Fe-HAP@PDA@CNT-NH 2 owned good loading efficiency on FA and had a wide applicability with different fertilizer slow release effects in different pH environments. Adsorption experiment revealed that Fe-HAP@PDA@CNT-NH 2 possessed high adsorption capacity for MB under different pH conditions. The pseudo-second order and Langmuir models discussed above can be utilized to describe the adsorption mechanism utilizing kinetic and isothermal adsorption models. In addition, the plant experiment also proved the effect of the composite soil conditioner on soil and plants. Hence, the new composite soil conditioner has a great promoting effect on soil improvement and crop growth.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Fawen Liang,Zhang Liu,Xueding Jiang,Jiesen Li,Kaibang Xiao,Weicheng Xu,Xin Chen,Jinzhi Liang,Zhifeng Lin,Meng Li,Xiaolian Wu,Hailong Wang
In this study, NaOH-modified biochar supported Fe/Mn bimetallic composite (Fe-Mn/AW-BC) was prepared to remove tetracycline (TC) through activating peroxymonosulfate (PMS). Results showed that about 97.9 % of TC was degraded and the rate constant of Fe-Mn/AW-BC + PMS system was 37 folds higher than BC + PMS system. Experimental results confirmed that both radical and non-radical pathway were contribute to the catalytic system. Density functional theory (DFT) results also suggested that Fe-Mn/AW-BC sample was favorable for adsorbing PMS based on the length O O bond from PMS and the E ads of catalysts. The superior activation ability was ascribed to the accelerating formation of reaction active species and other oxidation species by bimetallic structures of Fe-Mn and oxygenated functional groups of BC. Additionally, the redox cycles of Fe 3+ /Fe 2+ and Mn 3+ /Mn 2+ under Fe-Mn-BC synergism promoted the generation of the radicals, whereas the carbon shell effectively inhibited metals leaching of Fe-Mn/AW-BC, and 77.8 % of TC can be still removed within 60 min after five consecutive cycles. Notably, Fe-Mn/AW-BC system has special characteristic of wide pH usable range and broad-spectrum adaptability towards various organic pollutants and various water environments. Based on intermediate identification and Fukui function calculation, the degradation pathways of TC were also proposed. This study highlights the applications of biochar for the environmental catalysis.
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高影响因子
Science China-Chemistry
·
2021
·Vol. 64
·期 7
·1088-1095
·
IF 9.445
Zhai Liming,Zhang Bin,Liang Haojie,Wu Huibin,Yang Xinchun,Luo Gen,Zhao Shichao,Qin Yong
The design of efficient iron-based catalysts remains a great challenge for selective cyclohexane oxidation to cyclohexanone under mild conditions. Because of the complex distribution of iron location on the support, the selectivity is always low. Here, we report a general strategy to selectively deposit highly-dispersed FeO x into the micropore of ZSM-5 by atomic layer deposition (ALD). The framework of ZSM-5 and the Brønsted acid sites are intact during ALD, and the Fe species are selectively deposited onto the defect and Lewis acid sites of ZSM-5. Besides, more Fe-O-Si bonds are formed over FeO x /ZSM-5 with a low loading of Fe, while FeO x nanoparticles are generated at high Fe loading. They cannot be realized by the traditional solution method. The obtained FeO x /ZSM-5 catalysts perform high selectivity of cyclohexanone (92%–97%), and ALD cycle numbers of FeO x control the activity. Compared with the Fe nanoparticles, the Fe-O-Si species performs higher turnover frequency and stability in the oxidation reaction.
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高影响因子
ACS Catalysis
·
2020
·
IF 12.35
Xiaoli Yang,Ruifeng Wang,Jia Yang,Weixin Qian,Yaru Zhang,Xuning Li,Yanqiang Huang,Tao Zhang,De Chen
Direct conversion of syngas into aromatics with tandem catalysts containing Fe-based Fischer–Tropsch synthesis (FTS) catalysts and zeolites has been attracting significant attention because of the great cost-efficiency. However, the interaction role between two active species and reaction paths are still unclear. We report here that a high yield of aromatics was achieved by serial reactions directly from syngas on a Na-Fe-ZrO2/ZSM-5 tandem catalyst. Results point out significant impacts of zeolite in the catalytic system on performance including activity and selectivity. The role of the zeolite on reaction pathways about both CO conversion and aromatic formation has been systematically investigated by steady-state isotopic transient kinetic analysis and designed experiments. The presence of zeolite in the catalytic system promotes the CO hydrogenation rate by means of improving the iron carburization degree, possibly because of the enhanced CO adsorption and the formation of surface intermediates. It also enhances selectivity to aromatics by coupling CO to participate in the olefin transformation on ZSM-5. In addition, the formation rate of aromatics is proportional to the number of Lewis acidic sites, suggesting the dehydroaromatization route as the main mechanism of olefin aromatization. These findings provide some insights into the effect of ZSM-5 on reaction paths over the FTS catalyst–zeolite tandem catalyst system.
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高影响因子
NANOTECHNOLOGY
·
2017
·Vol. 28
·期 7
·075101
·
IF 3.44
Yunchun Zhou,Qian Liu,Xuping Sun,Rongmei Kong
The determination of specific nucleic acid sequences is key in identifying disease-causing pathogens and genetic diseases. In this paper we report the utilization of Fe-nitrilotriacetic acid coordination polymer nanowires as an effective nanoquencher for fluorescence-enhanced nucleic acid detection. The detection is fast and the whole process can be completed within 15 min. This nanosensor shows a low detection limit of 0.2 nM with selectivity down to single-base mismatch. This work provides us with an attractive sensing platform for applications.
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PubMed
高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Biao Hu,Bing-Hao Wang,Lang Chen,Zhang-Jun Bai,Wei Zhou,Jun-Kang Guo,Sheng Shen,Ting-Liang Xie,Chak-Tong Au,Li-Long Jiang,Shuang-Feng Yin
In the design of photocatalysts for ammonia synthesis, the construction of effective nitrogen (N2) adsorption and activation sites is critical. Herein, Fe single atoms were effectively fixed on the surfaces of WO2.72–x nanowires. Electronic interactions between single Fe atoms and WO2.72–x resulted in a d-band center shift toward the Fermi level and thus enhancement of N2 bonding with the catalyst surface. The studies of differential charge density and electron localization reveal that there is enhanced electron transfer from Fe-SA/WO2.72–x to the adsorbed N2, signifying that Fe single atoms are active centers for N2 activation. Benefiting from electronic interactions, the optimized catalyst shows a NH4+ generation rate of 186.5 μmol g–1 h–1 during photocatalytic N2 reduction.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Zhengwen Fan,Xinjiao Cui,Jiankun Wei,Chan Chen,Haolin Tang,Junsheng Li
Fe N C is the most promising material to replace the noble metal catalyst for cathodic oxygen reduction reaction in proton exchange membrane fuel cells (PEMFCs). However, the practical performance of Fe N C catalyst is significantly limited by its low active site (Fe-N 4 ) density. Herein, we propose to promote the formation of Fe-N 4 active sites in Fe N C catalyst by strengthening the interaction of N precursors and Fe precursors during the carbonization synthesis. In our approach, ionic liquid (IL, [EMIM][NTf 2 ]) with high nitrogen content and good thermal stability is caged in the pores of Fe-ZIF-8 through the host–guest interactions. These interactions are critical for the preservation of Fe and N species and formation of active sites during the synthesis. The optimal catalyst developed with this approach (Fe 0.05 N C/10) has a high density of accessible Fe-N 4 sites (1.88*10 19 sites g −1 ). Therefore, in both acidic and alkaline media, Fe 0.05 N C/10 showed excellent ORR activity comparable to commercial Pt/C catalyst. Moreover, PEMFC performance with a peak power density of 300 mW cm −2 was demonstrated with Fe 0.05 N C/10 under H 2 /O 2 conditions. The synthetic approach reported herein may be used for tailoring of advanced catalyst with high intrinsic activity.
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高影响因子
Nanomaterials
·
2022
·Vol. 12
·期 23
·4138
·
IF 5.719
Weihua Qin,Yueming Ma,Ting He,Jingbin Hu,Pan Gao,Shaoxia Yang
A heterogeneous Fenton-like catalyst with single redox site has a rate-limiting step in oxidant activation, which limited its application in wastewater purification. To overcome this, a bimetallic doping strategy was designed to prepare a heterogeneous Fenton-like catalyst (Fe-Mo/rGO) with a double-reaction center. Combined with electrochemical impedance spectroscopy and density functional theory calculation, it was confirmed that the formation of an electron-rich Mo center and an electron-deficient Fe center through the constructed Fe-O-Mo and Mo-S-C bonding bridges induced a higher electron transfer capability in the Fe-Mo/rGO catalyst. The designed Fe-Mo/rGO catalyst exhibited excellent sulfamethazine (SMT) degradation efficiency in a broad pH range (4.8–8.4). The catalytic performance was hardly affected by inorganic anions (Cl−, SO42−and HCO3−) in the complicated and variable water environment. Compared to Fe/rGO and Mo/rGO catalysts, the SMT degradation efficiency increased by about 14.6 and 1.6 times in heterogeneous Fenton-like reaction over Fe-Mo/rGO catalyst. The electron spin resonance and radical scavenger experiments proved that ·O2−/HO2· and1O2dominate the SMT removal in the Fe-Mo/rGO/H2O2system. Fe and Mo, as active centers co-supported on rGO, significantly enhanced the electron transfer between catalyst, oxidant, and pollutants, which accelerated the reactive oxygen species generation and effectively improved the SMT degradation. Our findings offer a novel perspective to enhance the performance of heterogeneous Fenton-like catalysts by accelerating the electron transfer rate in the degradation of organic pollutants.Keywords:heterogeneous Fenton-like reaction;Fe-Mo dual-reaction-center catalyst;reactive oxygen species;sulfamethazine
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PubMed
高影响因子
DYES AND PIGMENTS
·
2019
·
IF 4.018
Yingting Zheng,Hailong Wang,Jianzhuang Jiang
A fluorescent porous tetraphenylethylene-based organic polymer ( PTOP ) was constructed by the reaction of 5,5',5'',5‴-(ethene-1,1,2,2-tetrayltetrakis(benzene-4,1-diyl))tetrakis(pyrimidin-2-amine) and cyanuric chloride in the presence of potassium carbonate. CO 2 sorption experiment at 195 K reveals the permanent porosity of PTOP with a Brunauer-Emmett-Teller surface area of 227 m 2 g −1 . In particular, the existence of rich secondary amines and pyrimidine nitrogen atoms surrounding the 1,3,5-triazine moieties in PTOP provides abundant chelating sites for metal ions, endowing a fast-response and sensitive fluorescence sensing Fe(III) with a low limit of detection of 4.5 μM. In addition, this polymer also shows an excellent sensing performance towards nitrobenzene with good selectivity and a low detection limit of 1.6 nM.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 21
·8952-8959
·
IF 3.288
Hehe Qin,Jinhong Fan,Shun Mao
The Fenton method is an important water treatment process. However, the mechanism of the Fenton reaction is still not widely recognized. In this article, the autocatalysis process responsible for the degradation of 4-chlorophenol (4-CP) as well as the generation of Fe(II) and the decomposition of H2O2 is elaborated using a Fe(III)/H2O2 system. It was found that the one electron reduction of Fe(III) to Fe(II) via oxidization of H2O2 to ˙HO2 is not spontaneous according to the standard electrode potential rather than being limited by the rate constant of 0.0027 M−1 s−1 in view of the Haber–Weiss circulation. However, the reaction of Fe(III) and 4-CP is spontaneous with a second-order kinetic rate constant of >0.12 M−1 s−1 and a conversion rate of 0.56%, which triggers the switch of the Fenton-like reaction as a real rate-determining step. The circulation of Fe(III) to Fe(II) in the proposed Fenton-like reaction mechanism depends on the organic species and various intermediates, which indicates its reaction selectivity, preferable for organics with a stronger thermodynamic and kinetic activity. Besides, a slight pH decline with time-scale and the stoichiometric ratio of ˙OH to H2O2 and H2O2 to 4-CP being 1 and 2, respectively, pointed to the new proposed reaction mechanism. The discovery of the new reaction mechanism might promote the theoretical and technical advancement of the Fenton-like process.
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高影响因子
FUEL
·
2019
·
IF 5.128
Tengfei Yang,Congcong Liu,Chuan Li,Liyong Gan,Wenan Deng,Qingshan Niu
Nickel sulfide is regarded as one of the most promising substitutes for the best-performing disposable molybdenum catalyst in the hydrogenolysis of lignite and heavy residue, but its practical application is hindered severely by insufficient catalytic activity and a prohibitively large dosage. Herein, we report that the issues of activity and cost of nickel sulfide can be addressed simultaneously by employing a combination of iron incorporation and a dispersing strategy via oil-soluble ligands. Motivated by first-principles calculations where iron incorporation in nickel sulfide would lead to a better activity towards the rate-limiting step of hydrogenolysis compared with nickel sulfide alone, we successfully prepared a well-dispersed Fe-Ni-S catalyst by coordinating active metal salts with carboxylate ligands and a subsequent essential sulfurization. The synthesized Fe-Ni-S catalyst outperformed not only the monometallic nickel catalyst but also the commercial molybdenum catalyst in the hydrogenolysis of lignite and heavy residue, and exhibited a high conversion efficiency, hydrogen consumption, hydrogen/carbon product atomic ratio, and dispersibility of solid residues, with an economic nickel dosage of as low as ~250 μg·g −1 . Structural changes of raw coal and solid residues further confirmed the role of the Fe-Ni-S catalyst in facilitating the hydrogenolysis of lignite and heavy residue.
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高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Yibo Tang,Ying Lei,Kang Tong,Tong Yang,Tiantian Fu,Yang Xiang,Shulin Zhang,Yujun Si,Chaozhong Guo
Fe, N-doped graphene-like carbon layers-wrapped carbon black composite (L-Fe-AD+C) was developed by pyrolyzing the mixture of Fe-adenine precursors and conductive carbon black as an efficient catalyst to oxygen reduction reaction (ORR). Graphitic N sites with more ORR activity are preferentially formed due to the facilitation of metallic Fe. Furthermore, graphene-like ultra-thin networks wrapped around nanoparticles of carbon black greatly increase the exposure of active sites and construct continuous diffusion channels favorable for the transfer of substances. As a result, the as-prepared L-Fe-AD+C exhibits an excellent ORR activity in alkaline electrolyte with a high half wave potential (0.88 V), and superior selectivity together with admirable stability, which are comparable to those of the benchmark Pt/C catalyst. More encouragingly, the L-Fe-AD+C can serve as an efficient cathode catalyst in a zinc-air battery, which reaches a peak power density of 221 mW cm −2 approximating to that of Pt/C catalyst (236 mW cm −2 ). The battery also shows a steady discharge voltage plateau of 1.26 V and specific capacity of 799 mAh g −1 at a discharge current density of 10 mA cm −2 . The results suggest the considerable potential of the L-Fe-AD+C catalyst to replace precious metal catalysts.
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危险品化学品经营许可证（带存储）