ENVIRONMENTAL POLLUTION
·
2021
·
IF 8.071
Anqi Huang,Dan Zhi,Yaoyu Zhou
A graphite felt (GF) cathode was firstly modified by Fe–Mn binary oxide (FMBO), active carbon (AC), carbon black (CB), and polytetrafluoroethylene (PTFE), which exhibits satisfactory ciprofloxacin (CIP) removal efficiency at neutral pH value in electro-Fenton (EF) system. Morphological data showed that modified cathodes have larger surface area and volume pore as well as more active sites. And electrochemical properties have proved stronger current response after modification. In compassion to the unmodified GF, the FMBO/AC/CB modified GF (FMBO-GF) has wider pH range and higher CIP removal efficiency due to its unique nanoparticles structure. The CIP removal efficiency achieved 95.40% in 30 min, and the removal efficiency of total organic carbon (TOC) achieved 93.77% in 2 h when conditions were optimal (25 mg/L initial CIP concentration, 2 mA/cm 2 current density, FMBO/AC: CB: PTFE of 1:1:5, and 7 initial pH value) in this study. The results of great degradation and mineralization of CIP in this study indicate that the FMBO-GF cathode has huge potential on antibiotics removals in neutral environment.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 15
·9761-9770
·
IF 12.732
Dan Wang,Hao Xu,Peixia Yang,Lihui Xiao,Lei Du,Xiangyu Lu,Ruopeng Li,Jinqiu Zhang,Maozhong An
Extensive efforts have been devoted to active site designing for non-precious metal electrocatalysts; however, the porous structure engineering has been less emphasized, particularly for catalysts for gas diffusion electrodes, e.g., the cathode (oxygen reduction reaction, ORR) of Zn–air batteries. The desired porous structure is not only important for exposing high-density active sites but also beneficial for boosting mass transfer. Here, a dual-template strategy is proposed for constructing hierarchically porous structural Fe–N–C catalysts with dense active Fe–Nx moieties for the cathode of Zn–air batteries. The dual ZnCl2 and MgO hard templates jointly promote the formation of hierarchically interconnected carbon networks. The experimental results indicated both significantly improved active site accessibility and mass transfer, reasonably leading to enhanced ORR activity in conventional three-electrode cells. Particularly, it is deduced that the microporous structure is beneficial for dense active Fe–Nx moieties, while the ultra-macroporous structure is conducive to mass transfer during the ORR process. We further applied this dual-template-mediated catalyst in a real-world liquid Zn–air battery, which presents a high open-circuit voltage of 1.48 V and a remarkable energy density of 952.8 W h kgZn−1. Such robust battery performance is among the best compared with reported Zn–air batteries using non-precious metal catalysts. Particularly, a peak power density of 116.8 mW cm−2 is achieved in an all-solid-state Zn–air battery.
✓ 已验证
产品关联
DOI
高影响因子
ANALYST
·
2021
·Vol. 146
·期 14
·4557-4565
·
IF 4.616
Xiangyu Ma,Kun Qian,Onome Ejeromedoghene,Martha Kandawa-Schulz,Wei Song,Yihong Wang
Taking a composite of a nanomaterial and a signal molecule as a substrate material can provide a label-free electrochemical platform. Besides, the nanomaterial with a high catalytic activity towards the signal molecule can improve the sensitivity of the platform. Herein, a thionine functionalized Fe–N–C nanocomposite was employed as the substrate. Firstly, the electrocatalytic activity of Fe–N–C towards the electroreduction of thionine was explored. Then, an immobilization-free and label-free electrochemical platform for the determination of microRNA-21 based on Fe–N–C–thionine/Fe3O4@AuNPs was constructed. A magnetic glassy carbon electrode (MGCE) was used to keep the magnetic Fe–N–C–thionine/Fe3O4@AuNPs modified onto the surface of the MGCE. Fe–N–C and Fe3O4 nanoparticles can co-catalyze the electroreduction of thionine and a strong electrochemical reduction signal of thionine could be realized in the differential pulse voltammetry (DPV) test. Also, a catalytic hairpin assembly (CHA) reaction was utilized to enhance the sensitivity of the developed electrochemical biosensor. Besides, the developed biosensor shows excellent specificity and reproducibility in the test of human serum samples, indicating its wide application prospects in the early-stage diagnosis of tumors.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Wei Miao,Ying Liu,Dandan Wang,Ningjie Du,Ziwei Ye,Yang Hou,Shun Mao,Kostya (Ken) Ostrikov
Transition-metal and nitrogen co-doped carbon-based catalysts receive much attention in peroxymonosulfate (PMS) activation. However, the contribution of doped metal and the kinetic mechanisms of the emerging nonradical pathways especially enabled by reactive singlet oxygen species remain unclear. Herein, we report Fe-N-co-doped carbon-based catalysts (FeCNx) for peroxymonosulfate activation. The catalysts achieve fast removal of a broad spectrum of organic pollutants in a wide pH range without the common Fe leaching. Both catalyst surface-activated PMS complex (catalyst-PMS*), surface-bound radicals, and singlet oxygen are identified. The new mechanism is enabled by the Fe-Nx single-atomic-site that enhances the adsorption of PMS and facilitates the formation of catalyst-PMS*. The formation route of singlet oxygen species is elucidated for the first time for Fe, N-co-doped carbon-based catalysts with density functional theory simulation. This study reveals the intrinsic role of Fe-Nx site in catalysts and provides new insights into the origin and kinetics of non-radical pathways for peroxymonosulfate activation.
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 37
·22780-22788
·
IF 3.361
Xiaoyi Sun,Qingjie Liu,Shuai Liu,Xintang Zhang,Shanshan Liu
A series of MOx–Cr2O3–La2O3/TiO2–N (M = Cu, Fe, Ce) catalysts with nitrogen doping were prepared via the impregnation method. Comparing the low-temperature NH3-SCR activity of the catalysts, CeCrLa/Ti–N (xCeO2–yCr2O3–zLa2O3/TiO2–N) exhibited the best catalytic performance (NO conversion approaching 100% at 220–460 °C). The physico-chemical properties of the catalysts were characterized by XRD, BET, SEM, XPS, H2-TPR, NH3-TPD and in situ DRIFTS. From the XRD and SEM results, N doping affects the crystalline growth of anatase TiO2 and MOx (M = Cu, Fe, Ce, Cr, La) which were well dispersed over the support. Moreover, the doping of N promotes the increase of the Cr6+/Cr ratio and Ce3+/Ce ratio, and the surface chemical adsorption oxygen content, which suggested the improvement of the redox properties of the catalyst. And the surface acid content of the catalyst increased with the doping of N, which is related to CeCrLa/TiO2–N having the best catalytic activity at high temperature. Therefore, the CeCrLa/TiO2–N catalyst exhibited the best NH3-SCR performance and the redox performance of the catalysts is the main factor affecting their activity. Furthermore, in situ DRIFTS analysis indicates that Lewis-acid sites are the main adsorption sites for ammonia onto CeCrLa/TiO2–N and the catalyst mainly follows the L–H mechanism.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Yun Pei,Junxian Qin,Jun Wang,Yun Hu
A series of Fe-based metal organic framework derived materials were prepared by thermal treating MIL-100(Fe) in nitrogen atmosphere for adsorption removal of oxygenated volatile organic compounds (OVOCs) such as methanol, formaldehyde and acetone under dynamic conditions. The experimental results showed that the partially carbonized M-350 material obtained by calcining MIL-100(Fe) at 350 °C exhibited the best adsorption performance and high stability. The breakthrough adsorption capacity of M-350 for methanol was 61.5% higher than that of pure MIL-100 (Fe), and it was 24.7, 6.5 and 2.6 times higher than that of commercial activated carbon, ZSM-5 and SAPO-34 adsorbents, respectively. The excellent adsorption performance was attributed to the exposure of abundant coordinatively unsaturated iron metal sites acting as Lewis acid sites through high temperature calcination, which had a strong affinity for OVOCs. Meanwhile, a hierarchical porous structure and high specific surface area further promoted the adsorption. This work provides new insights into the further development of metal organic frameworks based functional materials for VOCs removal and purification.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Katam Srinivas,Yuanfu Chen,Bin Wang,Bo Yu,Yingjiong Lu,Zhe Su,Wanli Zhang,Dongxu Yang
Strategic design and fabrication of a highly efficient and cost-effective bifunctional electrocatalyst is of great significance in water electrolysis in order to produce sustainable hydrogen fuel in a large scale. However, it is still challenging to develop a stable, inexpensive, and efficient bifunctional electrocatalyst that can overcome the sluggish oxygen evolution kinetics in water electrolysis. To address the aforementioned concerns, a metal–organic framework-derived Fe-doped Ni3Fe/NiFe2O4 heterostructural nanoparticle-embedded carbon nanotube (CNT) matrix (Fe(0.2)/Ni-M@C-400-2h) is synthesized via a facile hydrothermal reaction and subsequent carbonization of an earth-abundant Ni/Fe/C precursor. With a novel porous nanoarchitecture fabricated by a Ni3Fe/NiFe2O4 heterostructure on a highly conductive CNT matrix, this catalyst exhibits exceptional bifunctional activity during water electrolysis over the Ni/Fe-based electrocatalysts reported recently. It delivers a low overpotential of 250 mV to achieve a current density of 10 mA/cm2 with a small Tafel slope of 43.4 mV/dec for oxygen evolution reaction. It requires a low overpotential of 128 mV (η10) for hydrogen evolution reaction and displays a low overpotential of 1.62 V (η10) for overall water splitting. This study introduces a facile and straightforward synthesis strategy to develop transition metal-based nanoarchitectures with high performance and durability for overall water-splitting catalysis.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Ruzhen Xie,Yanbin Jiang,Andac Armutlulu,Ziye Shen,Bo Lai,Hui Wang
In this work, cost-effective, magnetic carbon-supported Fe@Ti composite (Fe@Ti/Cs) with abundant active sites was synthesized by one-step carbothermal reduction of ilmenite with the assistance of microwave oven and utilized as a highly efficient persulfate (PS) activator for the wastewater purification. The coexistence of Fe 0/2+/3+ , Ti 3+/4+ and oxygen vacancies on Fe@Ti/Cs was found to favor for the electron transfer to PS, which facilitate the generation of reactive oxygen species (ROS). Catalytic experiment results showed that the Fe@Ti/C-4 produced from ilmenite/carbon with a mass ratio of 4:1 exhibited the best catalytic activation performance towards PS for the degradation of Rhodamine B (RhB). Usage of merely 0.12 g/L Fe@Ti/C-4 enabled the removal of 94.01% RhB (200 mg/L) within 30 min in the PS containing system, significantly outperforming ilmenite + PS (29.29%) and carbon + PS (49.91%) systems tested under the same conditions. The physico-chemical properties of the produced Fe@Ti/Cs before and after the reaction were carefully characterized. Radical scavenging experiments and electron paramagnetic resonance (EPR) analysis were carried out to better understand the underlying mechanism. The results indicate that oxygen vacancies in Fe@Ti/C-4 promoted the electron transfer and participated in the transition metal redox cycle to generate ROS in the PS-containing system, which was highly efficient for degrading RhB into small molecules and finally enabling mineralization. This work offers a new perspective for designing highly efficient and stable PS activators with long life derived from natural ore for environmental remediation.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Jawad Ali,Ajmal Shahzad,Jia Wang,Jerosha Ifthikar,Wenli Lei,Gebremedhin G. Aregay,Zhulei Chen,Zhuqi Chen
The slow transformation of Fe 3+ back to Fe 2+ restrict the practical application of Fe-based catalytic treatment of organic pollutants . Herein, we report a new findings of MgAl-MoS 4 to accelerate the redox cycle of Fe 3+ /Fe 2+ in Fe 3+ /PMS system. Based on the degradation of 4-chlorophenol (4-CP) profile, the rate constant of Fe 3+ /MgAl-MoS 4 /PMS system was 40 to 42 folds higher than MgAl-CO 3 /PMS, MgAl-MoS 4 /PMS and Fe 3+ /PMS respectively. Moreover, Fe 3+ /MgAl-MoS 4 /PMS system was superior both in the degradation efficiency of pollutants as well as in the stoichiometric efficiency of oxidants from the recently reported Fe 3+ /WS 2 /PMS, Fe 3+ /MoS 2 /PMS or other well-known nano-catalysts systems. This co-catalytic effect of MgAl-MoS 4 on the studied redox metals falls in the order of Fe 3+ > V 5+ > Cu 2+ > Mn 2+ ~Ag + . Furthermore, the Fe 3+ /PMS/MgAl-MoS 4 system shows smooth degradation over a wide pH (3.0–7.0) and complete stabilities in the recycled studies. Additionally, the presence of excessive amounts of inorganic anions or organic matters also did not influence the degradation profile. In mechanism studies, both the unsaturated S 2− and Mo 4+ of MgAl-MoS 4 were disclosed to fuel electron continuously during the reduction of Fe 3+ ions, and thus accelerate the rate limiting step (Fe 3+ /Fe 2+ ). Additionally, the layered structure, memory effect and suitable surface charge of LDH material also concentrates the reactants molecules and hence, the boosted effect of MgAl-MoS 4 was associated with the better adsorption of Fe 3+ ions, the faster PMS decomposition, and the acceleration of Fe 3+ /Fe 2+ redox cycle. This work indicates a breakthrough in the field of classical homogenous Fe/PMS system, offers the very first report on the role of Mo 6+ and S 2− to modulate the redox behaviour of homogenous Fe ions in persulfate based advanced oxidation processes .
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2020
·
IF 4.65
Quanli Hu,Bin Yue,Hongyang Shao,Fan Yang,Jinghui Wang,Yin Wang,Jinghai Liu
Lanthanum-based LaMO 3 (M = Fe, Co, Ni) perovskite nanofibers were effectively fabricated by electrospinning approach coupled with calcination process. The crystallinity, microstructures, morphologies, elemental compositions, and chemical bonding states of LaMO 3 perovskites were investigated in detail. The electrochemical properties of LaMO 3 perovskite nanofibers as supercapacitor electrodes and lithium-ion battery anodes were elucidated. The specific capacitances of LaFeO 3 , LaCoO 3 , and LaNiO 3 nanofibers were 183.6, 95.8 and 116.3 F g −1 at the current density of 1 A g −1 , respectively. The supercapacitive properties of LaMO 3 NFs had originated from the redox reactions of M 3+ /M 2+ . As lithium-ion battery anodes, LaMO 3 (M = Fe, Co, Ni) nanofibers exhibited the specific discharge capacities of 331, 646, and 92 mAh g −1 after 200 cycles, respectively. This research endowed the potential and competent candidates of the perovskite type lanthanum-based nanofibers for supercapacitor electrodes and lithium-ion battery anodes.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2020
·
IF 5.578
Liguang Dou,Mingkai Fu,Yuan Gao,Lei Wang,Cunji Yan,Tianzeng Ma,Qiangqiang Zhang,Xin Li
Direct hydrogenation of CO 2 to synthetic natural gas at a lower temperature remains a big challenge especially in the presence of H 2 S impurity. This contribution describes the synthesis, structure, morphology and doping effect of a series of robust catalysts for CO 2 methanation under resistive heating, based on Ni-layered double hydroxides (LDH) grown on porous and electrically conductive nickel foam (NF) derived structured catalysts. As a result, LaNi/NF showed the highest CO 2 conversion (55%) and CH 4 formation rate (631.5 mmol·g −1 ·h −1 ) at lower temperature of 250 °C and FeNi/NF gave the optimal conversion at 350 °C (75%, 860.9 mmol·g −1 ·h −1 ), which was superior to the most of recently reported Ni-based supported catalysts. We found that the CH 4 selectivity of the H 2 S (50 ppm) poisoned catalysts was significantly decreased and CO was verified as the main by-product. In this case, LaNi/NF and FeNi/NF still retained much higher conversion rate at 300 °C, 29.8% for LaNi/NF and 27% for FeNi/NF, than the almost deactivated unmodified Ni/NF with maximum 5% CO 2 conversion. The extraordinary activities can be explained as that the dopants can greatly strengthen the metal-support interaction and further enhance the reducibility of active metallic Ni, as XRD, HRTEM, TPR and XPS indicated. Besides of this, DFT calculations demonstrated that the existence of La can greatly promote CO 2 adsorption by lowering the adsorption barrier from 0.55 eV of pure Ni to 0.12 eV, and further inhibit the gaseous H 2 S from chemisorbing on the catalyst surface owning to the relatively unstable Ni-S bond.
✓ 已验证
产品关联
DOI
高影响因子
Nano Research
·
2020
·Vol. 13
·期 12
·3206-3211
·
IF 8.183
Zhang Meng,Hu Zheng,Gu Lin,Zhang Qinghua,Zhang Linghui,Song Qian,Zhou Wei,Hu Shi
A series of carbon-based binary single-atom catalysts of Fe and Ni coordinated by nitrogen are fabricated using a glucose-chelating method. Depending on the Ni/Fe content, they exhibit a wide-range of controllable CO/H 2 ratio from 0.14 to 10.86, which is meaningful to specific chemical processes. The durability of the catalyst is evaluated over an 8-hour period with no significant degradation of activity. The variation of the faradaic efficiency with Ni/Fe content is justified by density-functional-theory based calculation of the reaction barrier in both hydrogen evolution and CO 2 reduction reactions.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）