Cell Reports Physical Science
·
2022
·
IF 7.832
Yingdong Hao,Fang Mao,Jialin Shi,Yonghui Zhao,Luozhen Jiang,Nannan Sun,Lina Li,Wei Wei
New catalysts and product diversification of direct CH 4 conversion remain very challenging in catalysis. Here, we report FeO x /ZnO photo-catalysts for the conversion of CH 4 to liquid oxygenates with high yield (4,108 μmol·g cat −1 ·h −1 ) and nearly 100% selectivity. Based on the combinative results from X-ray photoelectron spectroscopy, X-ray absorption, electron paramagnetic resonance, radical quenching, and theoretical calculations, it is found that, in addition to the activation of CH 4 in the liquid phase, the presence of highly dispersed FeO 3 motifs in the ZnO lattice facilitates the formation of surface-active O − species; this plays an effective role for CH 4 activation to · CH 3 radicals. Meanwhile, HCHO is obtained as the major product in our system, rather than the typically reported CH 3 OH, and this may offer new opportunities to extend the product structure of CH 4 upgrading via tandem catalysis.
研究领域:
催化化学
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材料科学
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环境科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yujie Yan,Zhang Ling,Wen Shu,Tao Huang,Rich Crane
A novel three-dimensional electrokinetic remediation (3D EKR) system, with FeO x /granular activated carbon (GAC) composite constituting a third electrode was investigated for the removal of Cr from a real contaminated soil. Such third electrode particles were distributed evenly throughout the contaminated soil and their additional presence enabled the generation of a higher and more stable current density and reduced acid-base polarization of the soil, when compared against a conventional 2D EKR (cathode-anode) system. This resulted in a higher Cr removal, which was primarily driven by enhanced oxidation of Cr(III) to more mobile Cr(VI) aqueous complexes, which electromigrated towards the anode and into the anolyte. Analysis of FeO x /GAC and soil samples before and after EKR using XRD, FTIR, SEM-EDS, and XPS confirmed that: (i) both oxidation of Cr(III) and reduction of Cr(VI) occurred simultaneously on particle electrode surfaces; and (ii) aqueous Cr transport governed by electromigration was enhanced by Electro-Fenton reactions and hydrolysis on FeO x /GAC. A further benefit of 3D EKR was the promotion of residual Cr(III), in proximity to the cathode, to barely soluble crystalline silicate phases, therefore further decreasing the overall toxicity of the soil. This study therefore provides a highly promising first insight into the use of 3D EKR for the removal of Cr from contaminated land. Future work will seek to examine this emerging new technology at large scale and for different contaminated land scenarios, therefore further developing it towards a potential commercial application.
研究领域:
环境科学
·
土壤修复
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产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2019
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IF 4.309
Chunlei Wang,Qi Yao,Lina Cao,Junjie Li,Si Chen,Junling Lu
Preferential oxidation of CO in H2 (PROX) has been regarded as the most promising on-board approach to remove the trace levels of CO (∼1%) present in hydrogen fuels and thus to protect the Pt electrodes of proton exchange membrane fuel cells (PEMFCs) against CO poisoning. However, development of an active and selective catalyst toward CO oxidation in a broad low-temperature range remains challenging due to the competitive hydrogen oxidation reaction. Here, we report that selective deposition of the FeOx overcoat onto SiO2-supported Ir nanoparticles using the atomic layer deposition (ALD) technique allows precisely tailoring Ir–FeOx interfaces for optimizing catalytic performance in the PROX reaction. Compared to the uncoated Ir/SiO2 sample, FeOx-coated Ir/SiO2 samples exhibited remarkable activity enhancements, where we observed a volcano trend of the improved activity as a function of the numbers of FeOx ALD cycles. The optimized catalytic performance was achieved on a 1.5 nm Ir/SiO2 sample with two cycles of FeOx overcoating, by achieving complete CO conversion in a broad temperature range of 60–180 °C in the PROX reaction, which is the broadest temperature range over Ir-based catalysts reported in the literature so far. We noticed that the activity improvement over these samples was much less pronounced in CO oxidation in the absence of H2, which implies that the formation of hydroxyls on the FeOx overcoat might be attributed to the large activity enhancement in the PROX reaction.
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
DOI
高影响因子
INORGANIC CHEMISTRY
·
2025
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IF 4.7
Chao Yang,Hao Chen,Yuankai Li,Zhelin Su,Yeshuang Wang,Xufei Liu,Huiling Fan
The low sulfur selectivity of Fe-based H2S-selective catalytic oxidation catalysts is still a problem, especially at a high O2 content. This is alleviated here through anchoring FeOx nanoclusters on UiO-66 via the formation of Fe–O–Zr bonds. The introduced FeOx species exist in the form of FeIII and FeII. Therein the FeIII–O species are the predominant active sites for H2S-oxidation. The formed Fe–O–Zr bonds strengthen the redox cycle of FeIII/FeII through promoting electron transfer from Fe to Zr. The FeII–O species can activate molecular oxygen to oxidize H2S into elemental S, which accelerates the formation rate of atomic S, hindering its further oxidation into SO2. The combination of these factors empowers the catalysts, enabling 100% H2S conversion and 98.2% sulfur yield. The catalyst also has satisfactory stability with the sulfur selectivity only decreasing from 98.2% to 91.3% after the reaction going on 50 h. The decreased sulfur selectivity might be caused by the deterioration of pores and the deposition of elemental S on the surface. The former hinders the diffusion of sulfur oligomers timely from pores to the gas phase, while the latter is suspected to capture electrons to promote its further reaction with molecular oxygen.
研究领域:
化学工程
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
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IF 8.3
Yuntao Qi,Bin Zhang,Dengrong Xue,Hui Zhang,Xiaoning Liu,Zhi Liu,Shichao Zhao,Zhuo Li,Fanchun Meng,Yong Qin
The catalytic conversion of CO2 to CO through hydrogenation has emerged as a promising strategy for CO2 utilization, given that CO serves as a valuable C1 platform compound for synthesizing liquid fuels and chemicals. However, the predominant formation of CH4 via deep hydrogenation over Ru-based catalysts poses challenges in achieving selective CO production. High reaction temperatures often lead to catalyst deactivation and changes in selectivity due to dynamic metal evolution or agglomeration, even with a classic strong metal–support interaction. Herein, we have developed a FeOx/Ru/Rutile multilayer epitaxial structure by depositing a FeOx layer onto the epitaxially grown RuO2 nanolayers on the surface of rutile nanoparticles. This multilayer epitaxial structure transformed into a structure in which Ru nanoparticles were decorated with FeOx layers with ultrastable strong metal-support interaction (SMSI). Subsequently, the FeOx decoration on Ru nanoparticles effectively shifted the dominant product from CH4 to 95% CO during CO2 hydrogenation. Remarkably, this catalyst exhibits exceptional stability and can be operated stably at 550 °C for a long time without apparent deactivation. Compared with the dynamic changes observed in supported Ru nanoparticles, the interaction between Ru and FeOx maintains their electronic states at different reaction temperatures. Furthermore, this Ru–FeOx interaction inhibits H2 activation capability, CO adsorption, and subsequent hydrogenation of CO. The transformation strategy employed here, which utilizes initial multilayer epitaxial structures, can be applied to construct SMSI to enhance metal catalysts’ catalytic performance.
研究领域:
催化
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材料科学
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化学工程
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环境科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE
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2023
·Vol. 58
·期 13
·5773-5787
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IF 4.5
Qi Cheng,Wang Wen-Han,Zheng Jin-Fan,Jiang Li-Wen,Meng Chao,Liu Hong,Wang Jian-Jun
The recent advancement of nanocatalysis offers great promise for cancer therapy, and the development of efficient nanozymes for catalytic biological reactions is highly desirable, but still challenging. Herein, we report the synthesis of ultra-small FeO x nanozymes which is enabled by the introduction of Cu 2+ . The obtained nanozymes exhibit versatile catalytic activities integratively for effective cancer treatment. In particular, the as-synthesized nanozymes display pH-dependent peroxidase (POD)-like catalytic activity and approach the optimal performance at around pH = 4, endowing it with the possibility for the precise treatment of tumors with acidic microenvironment. Furthermore, the FeO x nanozyme possesses a promising glutathione (GSH) depleting capability and allows to reverse the abnormal GSH level in the tumor issues. Additionally, the fabricated nanozymes are able to catalyze the decomposition of hydrogen peroxide (H 2 O 2 ) to O 2 , allowing to alleviate the hypoxic environment of the tumors and improving the function of immune system for the treatment of tumors. More importantly, the FeO x nanozymes showed remarkable stability and maintained the enzymatic activity after six months in storage. Collectively, the FeO x nanozyme was demonstrated as a promisingly effective nanomedicine for tumor treatment by 4T1 cells, providing insight into the rational design of efficient nanozymes for cancer treatment. Graphical abstract
研究领域:
纳米医学
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癌症治疗
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生物化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Xin Li,Shengxiao Zhang,MingMing Zhang,Mingwu Yu,Hou Chen,Huawei Yang,Qiang Xu
A novel FeO X nanoparticles supported biomass activated carbon (BAC/FeO X ) composite was prepared through one-pot calcination method with FeCl 3 and cherry stone powder as precursors. The carbonization of biomass, reduction of Fe 3+ , and FeO X anchored on carbon substrate could be achieved at the same time. Characterization with transmission electron microscope (TEM) and scanning electron microscope indicated that nanoscale FeO X distributed uniformly on carbon substrate, and X-ray photoelectron spectroscopy, X-ray diffraction, and high resolution TEM characterization proved that the loaded FeO X was high crystallinity of Fe 3 O 4 and α-Fe 0 . Bisphenol A (BPA) was used to investigate the degradation performance of BAC/FeO X activating peroxydisulfate (PDS). The ratio of raw materials affected degradation efficiency of BPA intensively through the content, valence state, and dispersibility of FeO X nanoparticles, and the optimal material could degrade 20 mg/L BPA completely in 5 min at 0.1 g/L in the presence of 1 g/L PDS. Free radical determination and quenching experiments indicated that both SO 4 •− and •OH were involved in BPA degradation. The degradation pathway was proposed based on the identification of degradation intermediates. The facile synthesis method, high activation efficiency, and low-cost and environmental friendly raw materials made the BAC/FeO X -50 an alternative catalyst for organic pollution water treatment .
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Hejiao Zhang,Shuang Liu,Wei Ding,Chao Liu,Yaoyao Huang,Hong Li,Huaili Zheng
Advanced oxidation processes (AOPs) based on sulfite (S(IV)) activation are gaining recognition as a promising Fenton-like strategy, primarily due to their ability to generate potent radicals (e.g., SO 4 − and HO ). However, the existence and role of a non-radical-driven oxidation pathway in the S(IV)-mediated degradation of contaminants remain under debate. Herein, a magnetic iron-carbon composite (FeO x @C) was fabricated using the MOF-templated method and utilized as a stable photocatalyst to activate S(IV) under UVA light, achieving >93.6 % degradation of 20 μM ofloxacin (OFL) with a high degradation rate constant of 0.073 min −1 within 45 min. The catalyst’s porous carbon structure facilitated the transport of substrates to active sites and shortened the diffusion distance between reactive species and contaminants. Adsorbed S(IV) donated one electron to photo-generated holes and exposed Fe(III) sites with the formation of SO 5 − , which then followed two distinct pathways to produce radicals (SO 4 − ) and non-radicals (Fe(IV) and 1 O 2 ) responsible for OFL degradation. By leveraging the synergy of both radicals and non-radicals, this innovative oxidative system showcased robust anti-interference capacities and exceptional performance in degrading contaminants from complex water matrices. This study provides new insights into the significant role of non-radical species in S(IV)-mediated decontamination processes.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 23
·7018-7026
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IF 6.177
Fei Wang,Fuying Zhu,Enxiang Ren,Qiang Zhang,Guo-Ping Lu,Yamei Lin
The development of efficient and green synthetic strategies for N-heterocycle synthesis has always been a research hotspot in organic synthesis. A facile one-pot iron-catalyzed synthesis of quinazolines from alcohols in water has been disclosed for the first time, in which a N-doped carbon encapsulated Fe–FeOx material (Fe–FeOx@NC) is applied as a catalyst, and various quinazolines (25 examples, 62–99%) are synthesized. The iron nanoparticles wrapped by nitrogen-doped carbon layers in Fe–FeOx@NC with strong anti-poisoning ability is the main reason for the high performance in the reaction. This protocol offers several advantages including the use of air as an oxidant, water as a solvent, and recyclable iron as a catalyst and high atom and step economy.
研究领域:
有机化学
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催化
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Qi Shao,Xu Han,Kaixin Li,Wanbing Guan,Yihan Ling,Zhe Lv
Solid oxide electrolytic cells (SOECs) enable efficient electrochemical reduction of CO 2 into CO, providing a sustainable solution for greenhouse gas mitigation. Nevertheless, the scarcity of stable and highly active cathode materials for the real application of SOECs is a serious challenge. Herein, a novel self-assembled composed cathode of Ni co-doped (Pr 0.5 Sr 0.5 ) 0.95 Fe 0.9 Nb 0.1 O 3-δ -Gd 0.1 Ce 0.9 O 2-δ (PSFNNb-GDC) is proposed as an efficient CO 2 electrolysis. The NiFe/FeO x nanoparticles with a core–shell structure are uniformly deposited onto the surface of the PSFNNb-GDC cathode. La 0.8 Sr 0.2 Ga 0.8 Mg 0.2 O 3-δ (LSGM)-based single cell with NiFe/FeO x @PSFNNb-GDC cathode achieve excellent performance (1.33 A cm −2 at 850 ° [email protected] V) and stability (800 ° [email protected] V) in long-term operation. The performance enhancement original from increased surface oxygen vacancies and in situ formed FeNi@FeO x core–shell nanoparticles. This research highlights the potential of rational structural design of SOECs cathode materials in advancing the field of CO 2 utilization
研究领域:
材料科学
·
能源化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
·
2020
·
IF 3.687
Yang Zhong,Bo Zhou,Lijun Wang
Fe/FeO x embedded in LDH was prepared by reducing the pre-synthesized [Fe(C 2 O 4 ) 3 ] 3− anions intercalated LDH and used as a multi-functional catalyst for synthesis of C7-C9 compound via transfer hydrogenation between furfural (C5) and short-chain alcohols (C2-C4) and a subsequent aldol reaction of furfural with intermediate short-chain aldehydes in the absence of a homogeneous base with furfuryl alcohol as a byproduct. Screening reaction conditions, evaluation and improvement of the cyclic catalytic performance, and determination of catalytically active components were performed, and the results demonstrated that both high conversion and high selectivity to the C C bond forming product can be obtained under a non-oxidizing atmosphere of Ar or H 2 /Ar mixed gas, a reaction temperature of 140 °C and a reaction time of 4 h; the catalyst was easily deactivated during the cycle experiments, however, its catalytic stability can be effectively improved by depositing Ni with weak reducibility on the surface of Fe nanoparticles at the cost of reducing partial catalytic activity. Fe/FeO x together with LDH as a whole proved to be effective in catalyzing the transfer hydrogenation reaction and the support LDH imparted basic catalytic function to the composite realizing the aldol reaction in the absence of a homogeneous base.
研究领域:
催化化学
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材料科学
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Fu Yang,Liuzhu Zhou,Xuexue Dong,Wanyu Zhang,Shuying Gao,Xuyu Wang,Lulu Li,Chao Yu,Qian Wang,Aihua Yuan,Jin Chen
Visible-light-driven environmental contaminants control using 2D photocatalytic nanomaterials with an unconfined reaction–diffusion path is advantageous for public health. Here, cost-effective siliceous composite microsheets (FeSiO-MS) combined with two distinct refined α-Fe2O3 nanospecies as photofunctional catalysts were constructed via a one-pot synthesis approach. Through precise control of Fe2+ precursor addition, specially configured α-Fe2O3 nanofibers combined with FeOx cluster-functionalized siliceous microsheets of ∼15 nm gradually evolved from the iron oxide-bearing molecular sieve, endowing a superior light-response characteristic of the formed nanocomposite. The catalytic experiment along with the ESR study demonstrated that the produced FeSiO-MS showed reinforced photo-Fenton reactivity, which was effective for rapid phenol degradation under visible light radiation. Moreover, the phenol removal process was found to be regulated by the specially configured types and concentrations of iron oxides. Notably, the obtained composites exhibited a considerable visible-light-induced bactericidal effect against E. coli. The constructed FeSiO-MS nanocomposites as integrated and eco-friendly photocatalysts exhibit enormous potentials for environmental and hygienic application.
研究领域:
环境科学
·
材料科学
·
光催化技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）