Inorganic Chemistry Frontiers
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2023
·Vol. 10
·期 14
·4209-4220
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IF 7
Yujun Wu,Xiaoyang Wang,Bianbian Tian,Wei Shuang,Zhengyu Bai,Lin Yang
Optimizing the adsorption energy of intermediates by precisely modulating the coordination structure of single-atom M–Nx–C electrocatalysts to significantly improve the oxygen reduction reaction (ORR) performance still remains a great challenge. In this work, guided by density functional theory (DFT) calculations, an axial coordination FeN5 single-atom catalyst was constructed by way of an FeN4 species anchored with the N atom from nitrogen-doped graphene to promote the ORR catalytic performance. The special coordination structure of FeN5 can significantly optimize the adsorption of the reaction intermediate and reduce the overpotential of the ORR process compared to that of the FeN4 planar structure, which is commonly used. Hence, the constructed axial coordination FeN5 single-atom catalyst shows extraordinary ORR catalytic performance (Eonset/Ehalf-wave = 0.992/0.916 V vs. reversible hydrogen electrode (RHE), JL = 6.06 mA cm−2 and a 93.9% current retention after 15 h) and a maximum power density of 141 mW cm−2 in a zinc–air battery, which is superior to those of commercial Pt/C. These findings provide new insights into the construction of high-efficiency ORR catalysts from the design of a single atom coordination environment.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Aotian Gu,Kaiwei Chen,Xinyu Zhou,Chunhui Gong,Peng Wang,Yan Jiao,Ping Mao,Kai Chen,Jigen Lu,Yi Yang
Advanced oxidation processes based on high-valent metal species have attracted much attention due to their high reactivity and selectivity in degrading refractory organic pollutants, but the preparation of such catalysts remains a great challenge. Herein, FeCoCu-nitrogen-doped carbon (FeCoCu-NC), a trimetallic catalyst capable of producing high-valent metal species, was synthesized by direct carbonization of core–shell Metal-organic frameworks (MOFs). The rationally designed catalyst exhibited high catalytic activity in wide pH range and high resistance to common radical scavengers, anions and natural organics. The incorporation of Cu in FeCoCu-NC (TNC X ) not only enhanced the catalytic activity but also changed the activation mechanism of peroxymonosulfate (PMS) from a radical pathway to a non-radical pathway dominated by high-valent metal species. In addition, the TNC 5 /PMS system showed higher trichlorophenol (TCP) removal efficiency and PMS utilization compared to the radical-dominated FeCo-NC/PMS system and the 1 O 2 -dominated CoCu-NC/PMS system. This study provides a facile strategy to the preparation of advanced catalysts from multi-metal MOFs and is expected to provide guidance for the design of heterogeneous high-valent metal catalysts.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 27
·71088-71102
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IF 5.8
Fan Xinfei,Liu Na,Yang Jia,Yu Yueling,Xu Yuanlu,Song Chengwen,Liu Yanming
Persulfate activation is emerged as an alternative applied in environment remediation, but it is still a great challenge to develop highly active catalysts for efficient degradation of organic pollutants. Herein, a heterogeneous iron-based catalyst with dual-active sites was synthesized by embedding Fe nanoparticles (FeNPs) onto the nitrogen-doped carbon, which was used to activate peroxymonosulfate (PMS) for antibiotics decomposition. The systematic investigation indicated the optimal catalyst exhibited a significant and stable degradation efficiency of sulfamethoxazole (SMX), in which the SMX can be completely removed in 30 min even after 5 cycle tests. Such satisfactory performance was mainly attributed to the successful construction of electron-deficient C centers and electron-rich Fe centers via the short C-Fe bonds. These short C-Fe bonds accelerated electrons to shuttle from SMX molecules to electron-rich Fe centers with a low transmission resistance and short transmission distance, enabling Fe (III) to receive electrons to promote the regeneration of Fe (II) for durable and efficient PMS activation during SMX degradation. Meanwhile, the N-doped defects in the carbon also provided reactive bridges that accelerated the electron transfer between FeNPs and PMS, ensuring the synergistic effects toward Fe (II)/Fe (III) cycle to some extent. The quenching tests and electron paramagnetic resonance (EPR) indicated O 2 ·− and 1 O 2 were the dominant active species during the SMX decomposition. As a result, this work provides an innovative method to construct a high-performance catalyst to active sulfate for organic contaminant degradation.
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Journal of Environmental Sciences
·
2023
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IF 6.9
Chaomin Jia,Jianbing Wang,Huijiao Wang,Sichao Zhu,Xiaohui Zhang,Yuxiang Wang
Water fluoride pollution has caused non-negligible harm to the environment and humans, and thus it is crucial to find a suitable treatment technology. In this study, La-Fe@PTA adsorbent was synthesized for the defluoridation of mine water. The results showed that the optimum conditions for defluoridation by La-Fe@PTA were pH close to 7.0, the initial F − concentration of 10 mg/L, the dosage of 0.5 g/L and the adsorption time of 240 min. Compared with SO 4 2‒ , Cl ‒ , NO 3 ‒ , Ca 2+ and Mg 2+ , CO 3 2‒ and HCO 3 ‒ presented severer inhibition on fluoride uptake by La-Fe@PTA. The adsorption process fits well with the pseudo-second-order kinetic model and Freundlich model, and the maximum adsorption capacity of Langmuir model was 95 mg/g. Fixed-bed adsorption results indicated that fluoride in practical fluorinated mine water could be effectively removed from 3.6 mg/L to less than 1.5 mg/L within 130 bed volume (BV) by using 1.5 g La-Fe@PTA. Furthermore, the adsorbent still had good adsorption capacity after regeneration, which confirms the great application potential of La-Fe@PTA as a fluoride ion adsorbent. The mechanism analysis showed that La-Fe@PTA adsorption of fluorine ions is a physicochemical reaction driven by electrostatic attraction and ion exchange.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 27
·70827-70841
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IF 5.8
Hao Mengqi,Wu Wei,Habibul Nuzahat,Chai Guang,Ma Xiaoli,Ma Xiaoqian
Excessive phosphate content input into natural water can lead to the waste of resource and eutrophication. Biochar is a kind of low-cost adsorbent. However, its adsorption capacity for phosphate is low. In order to solve this problem, Fe compound-modified fly ash/cotton stalk biochar composites (Fe-FBC) were prepared through co-pyrolyzed fly ash and cotton stalk at 800℃, followed by infiltration of FeSO 4 solution. The samples were characterized by scanning electron microscopy, Brunauer–Emmett–Teller, X-ray diffraction, Fourier transform infrared spectroscopy, and zeta potential. After modification, the hydrophilicity and polarity of Fe-FBC increased. In addition, the pore volume, specific surface area, and surface functional groups were significantly improved. The adsorption behavior of Fe-FBC for the removal of phosphate from water can be well fitted by the pseudo-second-order kinetic and Sips isotherm adsorption model, with a maximum adsorption capacity of 47.91 mg/g. Fe-FBC maintained a high adsorption capacity in the pH range of 3–10. The coexisting anions (NO 3 − , SO 4 2− , and Cl − ) had negligible effects on phosphate adsorption. The adsorption mechanisms of Fe-FBC include electrostatic attraction, ligand exchange, surface complexation, ion exchange, chemical precipitation, and hydrogen bonding. Moreover, the desorption process of phosphate was investigated, indicating that the phosphate-saturated Fe-FBC could use as slow-release phosphate fertilizer. This study proposed a potentially environmental protection and recycling economy approach, which consists of recycling resources and treating wastes with wastes.
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Journal of Materials Chemistry B
·
2023
·Vol. 11
·期 25
·5898-5909
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IF 7
Mei Yang,Jun Yao,Borui Su,Nini Xin,Ting Zhou,Mingze Zeng,Chengheng Wu,Dan Wei,Jing Sun,Hongsong Fan
As nanozymes, carbon dots (CDs) have attracted increasing attention due to their remarkable properties. Besides general enzyme activity, their photoluminescence and photothermal properties have been explored rarely, whereas their synergistic effects might produce CDs-based nanozymes of high performance. Here, iron-doped CDs (Fe-CDs) with tunable fluorescence and enhanced peroxidase-like activity were designed to develop a novel “three-in-one” multifunctional platform to provide dual-mode/dual-target detection and near infrared (NIR)-assisted antibacterial ability. This proposed strategy for a H2O2 test exhibited a wide linear relationship with a low limit of detection (LOD) of 0.16 μM (colorimetric) and 0.14 μM (ratiometric fluorescent). Furthermore, due to the nature of cholesterol being oxidized to H2O2 by cholesterol oxidase, sensitive and selective detection of cholesterol was realized, and the LOD was 0.42 μM (colorimetric) and 0.27 μM (ratiometric fluorescent), surpassing that reported previously. This result suggested that Fe-CDs could be used for dual-mode quantification of large family of H2O2-producing metabolites, thereby paving the way for developing multi-mode sensing strategies based on nanozymes. Moreover, this platform showed synergistic effects for antibacterial application, indicating great prospects for bacterial killing as well as wound disinfection and healing. Hence, this platform could contribute to the construction of multifunctional CDs with high performance.
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Materials Advances
·
2023
·Vol. 4
·期 14
·2999-3009
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IF 5
Xu Jia,Xuetong Xu,Cong Liu,Fuying Wang,Liuxue Zhang,Shuyan Jiao,Genxing Zhu,Guomin Yu,Xiulian Wang
In order to avoid the issues causing weaknesses in the cumene method, a heterojunction catalyst based on Fe(II)-MOF/g-C3N4 was synthesized via in situ synthesis. The combination of Fe(II)-MOF and g-C3N4 was stable. With the synergistic effect of photocatalysis and the Fenton effect, the catalyst could achieve efficient direct hydroxylation of benzene to phenol. The yield and selectivity were 16.4% and 98.8% under the optimum conditions, respectively. And the catalytic activity of the heterojunction still sustained well after 5 reaction cycles. Hence, the explored photocatalysis-self-Fenton system could be applied in the field of direct hydroxylation of benzene to phenol.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yaoyu Zhou,Jianlong Wang
Developing high performance electrocatalysts for effective antibiotics elimination for heterogeneous electro-Fenton (Hetero-EF) process is still a challenge. This work synthesized iron/cobalt bimetallic N doped graphitic carbon cages (Fe x Co@NC) from ZIF-8@ZIF-67-Fe dual MOF composite for Cephalosporin C (CEP-C) degradation in the Hetero-EF system at a wide pH range. Results indicated that CEP-C degradation rate and total organic carbon (TOC) removal efficiency by Fe 40 Co@NC catalyst were as high as 82.45% (60 min) and 61.35% (240 min) at natural pH, respectively. The unique structure with FeCo bimetal encapsulated inside the N doped graphitic carbon cages enabled Fe 40 Co@NC to show excellent catalytic reactivity for H 2 O 2 activation. The generated M (•OH) and •OH all contributed to CEP-C degradation. The synergistic effects of Co 0 /Co 2+ /Co 3+ and Fe 0 /Fe 2+ /Fe 3+ cycles made Fe 40 Co@NC catalyst to continuously activate H 2 O 2 . Moreover, Fe 40 Co@NC catalyst showed good stability in consecutive cycles, and could still remain excellent reactivity when applied for CEP-C degradation from the real CEP-C fermentation residue supernatant. Furthermore, a possible CEP-C degradation pathway was proposed based on the identified intermediates.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
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IF 9.9
Jun Zhang,Lin Hao,Zitong Chen,Yongjun Gao,Huan Wang,Yufan Zhang
Owing to the high demand for clean and renewable energy technologies, several studies have focused on developing economically feasible, highly effective, and stable non-precious electrocatalysts for promoting the oxygen evolution reaction (OER). This development has stimulated an expansion of investigative quests and indicated the importance of advancing electrocatalytic research in this field. Through a facile and efficient method, Ni nanoparticles were uniformly embedded into nanoporous carbon nanorods (Ni-NCN), which are subsequently electrodeposited on CoFe-layered double hydroxide (LDH) nanosheets to produce highly efficient Ni-NCN/CoFe-LDH composites used for OER. The composite exhibited excellent catalytic activity toward OER owing to its low overpotential (ƞ10 mA = 280 mV), small Tafel slope (42 mV dec −1 ), and excellent durability. The Ni-NCN/CoFe-LDH catalyst exhibited higher OER activity owing to its uniformly dispersed Ni nanoparticles, large specific surface area, enhanced electron transport, and synergistic effect of multiple composites. Additionally, the enhanced synergistic effect of Ni-NCN promoted higher OER performance compared with Ni-undoped carbon nanorod/LDH, indicating that the Ni dopant and LDH significantly contributed to the overall OER performance. The synergistic effect of multiple composites significantly contributed to the excellent OER performance, indicating their potential as OER catalyst.
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FUEL
·
2023
·
IF 7.4
Fei Wang,Songyin Yu,Hui Xu,Junfeng Feng,Feihong Guo,Xiaoxiang Jiang,Jianchun Jiang
To solve the problem of harsh reaction conditions in lipid hydrogenation into fatty alcohol over Cu based bimetallic catalysts, the cheap Ni-base catalyst with high activity was synthesized. By using the hydrothermal method, the flower-like SiO 2 -ZrO 2 support was prepared. The Ni-Fe/SiO 2 -ZrO 2 catalyst was further prepared by the impregnation method and utilized in the fatty acid hydrogenation to produce fatty alcohol. Under the reaction conditions (240 °C, initial H 2 pressure: 2 MPa and reaction time: 3 h), the Ni-Fe/0.13SiO 2 -ZrO 2 catalyst attained 96.0% conversion and 86.4% fatty alcohol yield, much higher than that of Ni-Fe/ZrO 2 without SiO 2 (conversion 86.1% and fatty alcohol yield 61.9%). The high catalytic activity of Ni-Fe/0.13SiO 2 -ZrO 2 was ascribed to the increase of surface area, reduction of NiO grain size, and formation of flower-like morphology. The high selectivity to fatty alcohol over Ni-Fe/0.13SiO 2 -ZrO 2 was related to the increase of Lewis acidity (extra active sites) and the decrease of oxygen vacancy which weakened the adsorption of aldehyde (enol) on the catalyst and thus facilitated the formation of fatty alcohol.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 23
·64233-64245
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IF 5.8
Jin Qi,Dong Yingbo,Pan Hanlin,Lin Hai
It is challenging to separate the materials for treating arsenic contamination of soil and water from systems. The natural magnetite covered with Fe–Mn bimetallic (oxyhydr)oxide (Fe–Mn MSM) was effectively created in this study, and its potential use in removing As from water and soil was investigated. Batch adsorption studies showed that the As(V) adsorption on Fe–Mn MSM could achieve equilibrium after 120 min when the initial As(V) concentration was 39.85 mg/L. The calculated maximum adsorption of Fe–Mn MSM for As(V) was 17.94 mg/g at 20 °C. The mechanism of As(V) adsorption was confirmed to be a combination of ligand exchange and electrostatic attraction by the outcomes of FTIR analysis, SEM, and batch adsorption tests. Fe–Mn MSM can also be a successful amendment for cleaning up As-polluted soil. The 5% Fe–Mn MSM treatment group had the lowest exchangeable fraction of As (EX-As) concentration, 0.039 mg/kg (8.3% of initial EX-As), after 40 days. Magnetic separation could be used to quickly and completely recover the used Fe–Mn MSM from the soil. EX-As was present in higher concentrations on Fe–Mn MSM than that of the original soil. As a result, this work offers a strategy that may be put into practice to cheaply remove As from soil and water while also encouraging the reuse of natural magnetite. Graphical abstract
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MATERIALS SCIENCE AND ENGINEERING A-STRUCTURAL MATERIALS PROPERTIES MICROSTRUCTURE AND PROCESSING
·
2023
·
IF 6.4
He Zhang,Xiao-Chun Deng,Guo-Hua Zhang
In this study, high performance W–Mo–Cu–Ni–Fe alloy samples with additions of Mo (0–6 wt%), Ni and Fe (total content: 2.5 wt% and 5 wt%) were obtained through liquid-phase sintering at lower temperature, with the raw material of ultrafine W–Mo–Cu–Ni–Fe composite powder. Ultrafine W–Mo–Cu–Ni–Fe alloy powder with strong sintering activity and uniform composition was obtained by two-stage reduction means composed of carbothermic pre-reduction and hydrogen deep deoxidation steps. Significantly, the bonding ability of W/Cu phase interface and the wettability of two phases are greatly improved due to the presences of Ni and Fe. Moreover, the addition of appropriate Mo content was advantageous to the formation of W–Mo solid solution . All alloy samples achieved higher densification degrees to guarantee that the sintered blocks possess outstanding overall performances. Especially, by adjusting Ni/Fe ratio, the highest tension strength and elongation of were achieved by W-2wt.%Mo-1.75 wt%Ni-0.75 wt%Fe-27.5 wt%Cu sintered block, which were 567 MPa and 10.37%, respectively. Moreover, owing to the presences of W–Mo and Cu–Ni–Fe solid solutions, this alloy also had the highest microhardness and bending strength of 446 HV and 1473 MPa, respectively. As increasing Mo content from 0 wt% to 6 wt%, the compression strength of sintered blocks was improved, and failure strains of all the sintered blocks are close to 100%, respectively. However, even though the Cu matrix network structure is more evenly distributed as a result of the existences of added Ni and Fe, the electronic movement ability of the sintered blocks was reduced, leading to a significant decrease in conductivity.
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