ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Haidong Yang,Yang Liu,Yutong Luo,Shiqing Lu,Bitao Su,Jiantai Ma
Electrocatalytic nitrogen reduction reaction (NRR) represents a highly promising process to ammonia synthesis for artificial N2 fixation. However, the yield rate for NH3 production and Faradaic efficiency (FE) are still low, which greatly hinder its widespread applications. Until now, although a variety of catalysts, including single-atom catalysts, have been developed for NRR in the pursuit of suppressing hydrogen evolution reaction (HER) and the corresponding higher FE, the limited NH3 yield rate makes them uncompetitive for the synthesis of ammonia. Herein, we report a Fe single-atom catalyst anchoring on a nitrogen-doped carbon substrate (Fe SAC/N–C) as a highly efficient NRR catalyst. The catalyst achieves a high FE of 39.6% in 0.1 M KOH under room temperature, particularly a dramatically enhanced NH3 yield rate of 53.12 μgNH3 h–1 mgcat–1. The isotopic labeling (15N2) experiment confirms that the NH3 production completely originates from N2 reduction. Meanwhile, theoretical calculations and X-ray fine structure analysis reveal that the Fe–N3 coordination of Fe SAC/N–C is indeed responsible for the suppression of HER, particularly resulting in a maximum activation of NRR intermediates to produce ammonia with a high yield rate.
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Catalysis Science & Technology
·
2020
·Vol. 10
·期 19
·6583-6598
·
IF 5.721
Jialing Chen,Gang Peng,Wei Zheng,Wenbo Zhang,Li Guo,Xiaoqing Wu
A superior Fe-containing MCM-22 zeolite prepared by a one-pot synthesis method (OP-Fe/M22) showed excellent NH3 selective catalytic reduction (NH3-SCR) activity and almost 100% N2 selectivity in a wide temperature window (200–500 °C). To investigate the effects of preparation strategies on the NH3-SCR reaction, other three Fe/MCM-22 zeolites with similar iron content (4.4–4.8 wt%) were prepared by solid-state ion exchange (SSIE-Fe/M22), incipient wetness impregnation (IM-Fe/M22) and mechanical mixing (MM-Fe/M22) methods, respectively. Catalytic results in NH3-SCR demonstrate that OP-Fe/M22 gives significantly higher activity in the whole temperature range (100–550 °C) than the other three post-synthesized catalysts. As revealed by XRD, UV-vis, H2-TPR, NH3-TPD, and Py-IR experiments, OP-Fe/M22 has the highest concentrations of isolated Fe3+ species and acid sites, and the lowest concentration of Fe2O3 nanoparticles among the four catalysts, which ensures its highest activity in the NH3-SCR reaction. Besides, OP-Fe/M22 exhibits the higher activity both in NH3 oxidation and NO oxidation reactions than IM-Fe/M22, indicating the better NO oxidation ability and NH3 storage capacity of OP-Fe/M22 which also facilitates the NH3-SCR process. In contrast with Cu-based MCM-22 zeolite obtained from the incipient wetness impregnation method at similar metal content (5% Cu/M22), OP-Fe/M22 shows comparable activity with 5% Cu/M22 in the low-temperature range (100–300 °C) while obviously higher activity at high temperatures (300–550 °C). Moreover, by removing part of undesired iron oxides in OP-Fe/M22 through mild acid post-treatments, the NH3-SCR activity of OP-Fe/M22 in the medium and high temperature ranges (200–550 °C) can be further improved, suggesting that OP-Fe/M22 is a potential catalyst with highly-efficient NH3-SCR activity in a wide temperature window.
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ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Qingqing Zha,Mingxia Li,Zihao Liu,Yonghong Ni
Metal–organic frameworks (MOFs) have attracted much interest in electrocatalysis as promising catalysts in recent years. However, it still remains a challenge to directly use MOF-based materials as bifunctional electrocatalysts for overall water splitting. Herein, a hierarchical Co,Fe-MOF-74/Co/carbon cloth (CC) three-layer hybrid electrode is synthesized by a simple electrochemical deposition technology with subsequent solvothermal treatment. Electrochemical performance investigations show that the as-constructed Co,Fe-MOF-74/Co/CC electrode exhibits impressive electrocatalytic activity for full water splitting, which only requires a low overpotential of 226 mV@20 mA cm–2 for the oxygen evolution reaction (OER) and 94 mV@–10 mA cm–2 for the hydrogen evolution reaction (HER), respectively. Employing the as-constructed electrode as the anode and cathode in a two-electrode setup simultaneously, only 1.65 V of the voltage is needed to deliver the current density of 20 mA cm–2. The above excellent electrochemical performances should be attributed to the specific architecture, the synergistic effect of the Co and Fe species, and the superhydrophilic surface of the catalyst. More importantly, further investigations uncover that metal hydroxides and oxyhydroxides produced in situ during electrochemical tests are the veritable active species, which promote the high catalytic activity of the present catalyst.
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Nano Research
·
2020
·Vol. 13
·期 1
·273-281
·
IF 8.183
Zhang Tao,Jiang Zhenqi,Chen Libin,Pan Chunshu,Sun Shan,Liu Chuang,Li Zihou,Ren Wenzhi,Wu Aiguo,Huang Pintong
As nanomedicine-based clinical strategies have continued to develop, the possibility of combining chemotherapy and singlet oxygen-dependent photodynamic therapy (PDT) to treat pancreatic cancer (PaC) has emerged as a viable therapeutic modality. The efficacy of such an approach, however, is likely to be constrained by the mechanisms of drug release and tumor oxygen levels. In the present study, we developed an Fe(III)-complexed porous coordination network (PCN) which we then used to encapsulate PTX (PCN-Fe(III)-PTX) nanoparticles (NPs) in order to treat PaC via a combination of chemotherapy and PDT. The resultant NPs were able to release drug in response to both laser irradiation and pH changes to promote drug accumulation within tumors. Furthermore, through a Fe(III)-based Fenton-like reaction these NPs were able to convert H 2 O 2 in the tumor site to O 2 , thereby regulating local hypoxic conditions and enhancing the efficacy of PDT approaches. Also these NPs were suitable for use as a T 1 -MRI weighted contrast agent, making them viable for monitoring therapeutic efficacy upon treatment. Our results in both cell line and animal models of PaC suggest that these NPs represent an ideal agent for mediating effective MRI-guided chemotherapy-PDT, giving them great promise for the clinical treatment of PaC.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2019
·
IF 6.393
Zhen Song,Yang Li,He Teng,Caifeng Ding,Guiyun Xu,Xiliang Luo
Herein, an antifouling and sensitive electrochemical enzyme sensing platform was developed based on a self-designed zwitterionic peptide and sacrificial iron metal-organic framework (Fe-MOF). The designed zwitterionic peptide was hydrophilic and neutral in charge, and it was used to improve the antifouling capability of the sensing system. Fe-MOF with amine groups was loaded with Au nanoparticles and further functionalized with a specific DNA sequence, and it was used as a sacrificial label. The sensing target, T4 polynucleotide kinase (PNK), can catalyze the 5′-hydroxyl termini of a unique hairpin DNA to phosphate group, and the hairpin DNA can then be hydrolyzed by lambda exonuclease (λ-Exo) and release a single nucleotide. In the presence of the released DNA sequence, a sandwich-type hybridization reaction was triggered, and the DNA linked Fe-MOF was selectively attached to the electrode surface, which can react with K 4 Fe(CN) 6 to form the electroactive Prussian blue and generate significantly enlarged current response. Based on the antifouling peptide and the sacrificial Fe-MOF, the biosensor exhibited satisfying analytical performance for the detection of T4 PNK, with a wide linear range from 1.0×10 −3 to 10 U·mL -1 and a low detection limit of 3.5×10 -4 U·mL -1 . Moreover, the biosensor was capable of effectively eliminating nonspecific protein adsorption and assaying target in human serum, indicating its promising potential for practical application.
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Advanced Healthcare Materials
·
2019
·Vol. 8
·期 23
·1900911
·
IF 6.27
Peng Ji,Haiqin Huang,Shirui Yuan,Le Wang,Siqi Wang,Yiwei Chen,Na Feng,Hanitrarimalala Veroniaina,Ziheng Wu,Zhenghong Wu,Xiaole Qi
Reactive oxygen species (ROS)-mediated apoptosis is considered a crucial therapeutic mechanisms for artesunate (AS). As an Fe(II)-dependent drug, the anticancer effect of AS is often limited due to insufficient Fe(II) concentration in targeted cells. To overcome this problem, a recombinant apoferritin nanocarrier containing ferriferous oxide (M-HFn) is constructed to produce auxiliary exogenous Fe(II) when delivering AS to cancer cells. Here, the newly fabricated AS-loaded M-HFn nanoparticles (M-HFn@AS NPs) can significantly improve the tumor-specific targeting and intracellular uptake efficiency of AS in human cervical carcinoma cells. After being captured in the acidic cavity of endosomes, M-HFn@AS NPs can simultaneously release Fe(II) and allow AS to activate satisfactory ROS-mediated apoptosis. Furthermore, in vivo studies demonstrate that M-HFn@AS NPs can selectively accumulate in tumors to efficiently inhibit tumor growth. Thus, M-HFn@AS NPs are a promising system to enhance the therapeutic effect of Fe(II)-dependent drugs.
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PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2019
·
IF 5.026
Ying Li,Yijie Han,Wei Li,Yuxin Li,Deyun Zhang,Yeqing Lan
A novel magnetic sulfur-doped Fe–Cu–Y trimetal oxide (MST) nanomaterial was successfully synthesized by a chemical coprecipitation method to remove As(III) via simultaneous oxidation and adsorption and then characterized by BET, VSM, FESEM, XPS, and FTIR techniques. The effect of solution initial pH on the adsorption of As(III), and the adsorption kinetics and isotherm were investigated in detail. The results indicated that the MST nanoparticles exhibited an excellent performance for As(III) removal in a pH range of 7–10 and were easily separated from aqueous solution with a magnet. The maximum removal capability for As(III) reached 202.0 mg/g at pH 7.0. The adsorption of As(III) was well fitted by the pseudo-second-order kinetic model and Langmuir isotherm model, respectively. The investigation of mechanism revealed that As(III) could be oxidized to As(V) by O 2 − and OH free radicals, generated via the dissolved O 2 obtaining an electron from Cu(I) on the surface of the adsorbent and Fenton/Fenton-like reaction, respectively. Meanwhile, the produced As(V) was adsorbed onto the surface of the nanoparticles through the electrostatic attraction or diffusion. The adsorbed As(V) further interacted with –OH groups via ion exchange or with Y(III) on the surface of the adsorbent to form a precipitate. Therefore, the MST nanoparticles are promising for the removal of arsenic from water.
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ADVANCED POWDER TECHNOLOGY
·
2019
·
IF 3.25
Lihua Gao,Zhenggen Liu,Yuzhu Pan,Cong Feng,Yang Ge,Mansheng Chu
Carbothermal reduction followed by magnetic separation has been recognized as an effective recovery strategy to achieve separation of Mn and Fe from ferruginous manganese ores (Fe-Mn ores). However, it is difficult to improve the recovery of manganese more than 85% by changing carbothermic roasting reduction and magnetic separation. This work clarified the underlying reason for the poor separation with the magnetic separation process and proposed a promising process for the recovery of Fe and Mn from Fe-Mn ore. The effect of operating variables on recovery and separation of Mn and Fe from Fe-Mn ore is initially investigated during the carbothermic reduction roasting process followed by magnetic separation to reveal the underlying reason for the poor separation from Fe-Mn ores. Then, the stepwise reduction behaviors of the MnO-Fe 2 O 3 and MnO-Fe 2 O 3 -Al 2 O 3 systems were investigated to clarify that the formation of composite oxide Mn 1−x Fe x O (0 < x < 0.497) and hercynite (FeO·Al 2 O 3 ) directly caused the poor separation of Fe and Mn from high-alumina Fe-Mn ores. Then, the stepwise reduction roasting behaviors of Mn 1−x Fe x O and FeO·Al 2 O 3 were investigated by XRD, SEM-EDS and XPS analysis. After adjusting the experimental parameters, iron-rich products with a Fe recovery of 94.31% and a grade of 85.21% and manganese-rich product with a Mn recovery of 90.05% and a grade of 54.35% are obtained. The mass ratio of Mn/Fe increased to 8.5 in the manganese-rich product.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2019
·Vol. 27
·期 5
·5085-5096
·
IF 2.914
Li Haijie,Huang Guofu,Wang Mianmian
2,2′,4,4′-Tretrabromodiphenyl ether (BDE47) is known as a typical polybrominated diphenyl ethers (PBDEs) due to its high environmental abundance, ecological toxicity, and bioaccumulation. In this study, the influences of three typical surfactants (CTAB, SDS, and TX-100) on BDE47 solubilization and degradation by the polyanionic cellulose–stabilized Pd/Fe (PAC-Pd/Fe) nanoparticles were investigated. The results showed that BDE47 solubilities increased linearly when surfactant concentrations were above their critical micelle concentrations (CMCs), and the solubilization capacities of surfactants for BDE47 followed the order of TX-100 > CTAB > SDS. The appropriate dosages of surfactants were favorable for BDE47 degradation due to enhancing solubilization and accelerating mass transfer, while excessive surfactants inhibited BDE47 degradation due to excessive and thicker micelles formed, but still higher than no surfactant. The influences of various factors (PAC-Pd/Fe nanoparticle dosage, solution pH, and temperature) on BDE47 degradation in TX-100 solution were also tested. The results showed that BDE47 degradation followed the pseudo first-order kinetics model. The degradation rates of BDE47 increased as PAC-Pd/Fe nanoparticle dosage and temperature increased. Weak acidic condition (pH 5.5) was favorable for BDE47 degradation with 96.8% BDE47 was removed within 7.5 min, while alkaline condition (9.0) was not conducive to the degradation of BDE47. The degradation of BDE47 by PAC-Pd/Fe nanoparticles was a catalytic reductive debromination process via active H-species attack, wherein the sequential debromination was the dominant reaction. This study suggests that in the presence of moderate surfactant, PAC-Pd/Fe nanoparticles may be potentially employed to eliminate BDE47 in contaminated water.
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高影响因子
Metals
·
2022
·Vol. 12
·期 12
·2050
·
IF 2.695
Yongfeng Li,Yanzhen Liu,Shuai Chen,Xiaoming Li,Shengguo Ma
A FeNx-C-based catalyst is considered one of the most promising candidates for the highest oxygen reduction reaction (ORR) activities among nonprecious metal-based electrocatalysts. In this work, a unique catalyst of nitrogen-doped twisted macroscopic graphene tubes decorated with Fe-Nx and bamboo-like carbon nanotubes (CNT) was prepared by using twisted iron wire as a template and cyanamide as a carbon source. The microstructure and physicochemical natures of the samples were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopic (XPS), X-ray diffraction (XRD), and nitrogen adsorption/desorption measurements. Torsion can promote the dislocation of the iron wire lattice, and activate the surface Fe atoms, thus leading to the growth of bamboo-like carbon nanotubes and forming iron nitride. The product has a graphene-like macroscopic tube structure and exhibits excellent ORR activity. Such excellent ORR performance may be ascribed to the synergistic effect, including high ORR catalytic sites caused by the dislocation of the iron wire lattice, nitrogen heteroatoms doping, favorable reactant transport channels provided by macroscopic tube structure, and fast electron transfer rate induced by 3D continuous networks.Keywords:twisted iron wires;catalyst;graphene tube;electrocatalytic activity
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CELLULOSE
·
2022
·Vol. 30
·期 2
·1171-1191
·
IF 6.123
Tu Chao,Sun Zenghui,Huang Fei,Wu Ziwei,Chen Hang
The photocatalytic process is an energy-saving and high-efficiency wastewater treatment technology. In this work, a simple in-situ hydrothermal method was used to prepare a photocatalytic material based on waste loofah with high efficiency, reusability and excellent heterostructure to improve the photodegradation efficiency. The prepared MoS 2 @MIL-101(Fe)@Carboxylated loofah composite material was characterized by scanning electron microscope (SEM), electrochemical impedance spectroscopy (EIS), UV–Vis diffuse reflection spectroscopy (UV–vis DRS), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), and transient photocurrent (TPC). The composite material demonstrated high adsorption capacity for hydrochloride (TC) and methylene blue (MB) and photocatalytic capacity under visible-light irradiation at room temperature which were attributed to the porous structure, strong visible-light absorption, and low recombination velocity of electron–hole pairs due to the heterojunctions. The loofah sponge used as a substrate can provide a means for powder catalyst recovery and waste cellulose recycling. Meanwhile, the photocatalyst proved excellent stability in the MB degradation experiment and could be reused for four cycles.
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Materials Today Energy
·
2022
·
IF 9.257
Xianglei Liu,Changjian Yuan,Hangbin Zheng,Chao Song,Cheng Tian,Ke Gao,Nan Sun,Zhixing Jiang,Yimin Xuan,Yulong Ding
Calcium carbonate (CaCO 3 ) pellets are suitable for scalable solar thermochemical energy storage but suffer from low solar absorptance, poor stability, and slow reaction kinetics, which lead to low solar energy storage efficiency. Here, for the first time, we successfully achieve fast and efficient solar thermochemical energy storage via synergistically employing Al, Mn, and Fe stabilizers for improving both cyclic stability and solar absorptance, and Li 2 CO 3 promoters for accelerating decomposition of CaCO 3 pellets. The average solar absorptance is 1500% higher than that of pure CaCO 3 pellets. After 60 cycles, the energy storage density is still as high as 1671 kJ/kg with a decay rate of only 4.14%, in stark contrast to energy density of 1121 kJ/kg and decay rate of 56.73% for pure CaCO 3 pellets. The average decomposition rate is about twice as fast as that of pure CaCO 3 pellets due to enhanced Ca 2+ diffusion by doped Li 2 CO 3 . Under direct light irradiation, novel CaCO 3 pellets demonstrate high energy storage rate due to both high solar absorptance and fast decomposition rate, while pure CaCO 3 pellets cannot even reach the decomposition temperature. This work opens new opportunities for scalable deployment of direct solar-driven thermochemical energy storage techniques based on Li 2 CO 3 -doped dark CaCO 3 pellets.
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