INORGANIC CHEMISTRY COMMUNICATIONS
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2023
·
IF 3.8
Chuncheng Shi,Zhixin Zhao,Ling Zhao,Aparna Kushwaha,Abhinav Kumar,Jun Wang,Ying Pan,Mohd. Muddassir,Qian Lan
Organic dyes are typical chemical reagents that find applications in printing, textile, leather, and other industries. However, their overuse and uncontrolled discharge in water bodies have a negative impact on the aquatic ecosystem and humans. Metal-organic frameworks are assorted multifunctional materials that find potential application as photocatalysts. In this work, the application of two porphyrin-based metal-organic frameworks (TCPP-La and Fe-TCPP-La) have been reported as photocatalytic materials to degrade dyes methyl orange (MO) and methylene blue (MB). The results suggest that TCPP-La can eliminate 16 % MO and 23.7 % MB in 125 min under UV irradiation of 385 nm. On the other hand, only 4.8 % MO and 16 % MB were removed by Fe-TCPP-La under the same condition. However, when hydrogen peroxide (2 % H 2 O 2 ) was added to the reaction medium, the degradation activity of TCPP-La was improved upto 26 % for MO and 61 % for MB, while, Fe-TCPP-La exhibits more enhancement in photocatalytic degradation upto 55 % for MO and 93 % for MB. The result implied that introducing ferric ions using post-synthetic strategy to engender both lanthanum and iron centers into the framework could improve the photocatalytic performance of the MOF against dye photodegradation.
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International Journal of Environmental Research and Public Health
·
2023
·Vol. 20
·期 5
·4571
·
IF 4.614
Shuyan Yu,Huiying Zhang,Congju Li
In this study, MIL-53(Fe) was innovatively incorporated into carbon felt (CF) by growing in-situ using the solvothermal method. MIL-53(Fe)@carbon felt (MIL-53(Fe)@CF) was prepared and used for the degradation of rhodamine B (RhB). As a new photocatalytic membrane, MIL-53(Fe)@CF photocatalytic membrane has the characteristics of high degradation efficiency and recyclability. Influence of various parameters including MIL-53(Fe)@CF loading, light, electron trapper type, and starting pH on RhB degradation were investigated. The morphology, structure, and degradation properties of MIL-53(Fe)@CF photocatalytic membrane were characterized. Corresponding reaction mechanisms were explored. The results indicated that pH at 4.5 and 1 mmol/L H2O2, 150 mg MIL-53(Fe)@CF could photocatalytically degrade 1 mg/L RhB by 98.8% within 120 min, and the reaction rate constant (k) could reach 0.03635 min−1. The clearance rate of RhB decreased by only 2.8% after three operations. MIL-53(Fe)@CF photocatalytic membrane was found to be stable.Keywords:MIL-53(Fe)@carbon felt;photocatalytic;degradation;rhodamine B
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JOURNAL OF POWER SOURCES
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2023
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IF 9.2
Yabiao Pei,Weikang Zhu,Runfei Yue,Jie Yao,Xin Liu,Lianqin Wang,Junfeng Zhang,Yan Yin,Michael D. Guiver
Adjusting catalyst/ionomer agglomerate is crucial to a high-performance catalyst layer (CL), particularly for non-precious metal catalysts . As a sacrificial component, the solvent plays a vital role during the CL formation process and resulting microstructure, determining the performance of the anion exchange membrane fuel cells (AEMFCs). Here, solvent mixtures of isopropanol (IPA) and tetrahydrofuran (THF) are studied for the controllable construction of the Co/Fe–N–C CL. The results indicate that the aggregate state of the ionomers and catalysts and the final CL microstructure strongly depend on the ratio of IPA and THF. The CL prepared with IPA: THF = 1:2 (v/v) shows a homogeneous distribution of Co/Fe–N–C catalysts, embedded in the ionomer matrix, due to the fast volatilization and low viscosity of the catalyst ink. The Co/Fe–N–C CL with high moisture adsorption behavior and retention ability results in a high performance AEMFC with peak power density of 545.3 mW cm −2 at 80 °C. The obtained results can guide the rational design of microstructure in non-precious metal CLs for high-performance AEMFCs.
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Analytical Methods
·
2023
·Vol. 15
·期 19
·2334-2342
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IF 3.1
Qian Li,Jing Yang,Wenzhan Yu,Liqiong He,Renlong Zhou,Changming Nie,Lifu Liao,Xilin Xiao
Monocrotophos (MP), an organophosphorus pesticide, poses a serious threat to human health, so a rapid and simple technique is needed to detect it. In this study, two novel optical sensors for MP detection were created using the Fe(III) Salophen complex and Eu(III) Salophen complex, respectively. One sensor is an Fe(III) Salophen complex (I-N-Sal), which can bind MP selectively and form a supramolecule, resulting in a strong resonance light scattering (RLS) signal at 300 nm. Under the optimum conditions, the detection limit was 30 nM, the linear range was 0.1–1.1 μM, the correlation coefficient R2 = 0.9919, and the recovery rate range was 97.0–103.1%. Interaction properties between the sensor I-N-Sal and MP and the RLS mechanism were investigated using density functional theory (DFT). And another sensor is based on the Eu(III) Salophen complex and 5-aminofluorescein derivatives. The Eu(III) Salophen complex was immobilized on the surface of amino-silica gel (Sigel-NH2) particles as the solid phase receptor (ESS) of MP and 5-aminofluorescein derivatives as the fluorescent (FL)-labeled receptor (N-5-AF) of MP, which can selectively bind the MP and form a sandwich-type supramolecule. Under the optimum conditions, the detection limit was 0.4 μM, the linear range was 1.3–7.0 μM, the correlation coefficient R2 = 0.9983, and the recovery rate range was 96.6–101.1%. Interaction properties between the sensor and MP were investigated by UV-vis, FT-IR, and XRD. Both sensors were successfully applied to the determination of MP content in tap water and camellia.
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Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Huihu Wang,Hao Tu,Feng Chen,Huang Xu,Ziguan Zhang,Guode Chen,Chenhuinan Wei,Xing Xiang,Zhixiong Xie
Through a facile oil bath method, a novel highly dispersed NH 2 -MIL-101(Fe)/carboxylated g-C 3 N 4 (NM-101(Fe)/CCN) heterostructure was prepared using the chemical bonding between carboxyl groups and -NH 2 groups. Compared with the octahedral morphology of pure NM-101(Fe), the chemical bonding interaction promoted the heterogeneous nucleation and growth of NM-101(Fe) to form nanometer-sized granular morphology, which was homogeneously dispersed on CCN surface. Cr(Ⅵ) and ciprofloxacin (CIP) were selected as the typical pollutant models in micro-polluted water sources. The results showed that 10 %NM-101(Fe)/CCN heterostructure could remove 97 % of Cr(Ⅵ) in 60 min and 88 % of ciprofloxacin (CIP) in 120 min. In the dual pollutant system of Cr(Ⅵ) and CIP, Cr(Ⅵ) reduction and CIP degradation can promote each other, and the degradation efficiency of CIP reached 96 % within 120 min. The apparent rate constant of 10 %NM-101(Fe) /CCN heterostructure for Cr(Ⅵ) reduction was 4.30 and 9.67 times of that of NM-101(Fe) and CCN, respectively, which may be ascribed to the interface electric field and good interface bonding of heterojunction . The charges separation efficiency was significantly improved, which effectively enhanced the photocatalytic activity.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·
IF 19
Le Xiang,Daochuan Jiang,Yue Gao,Chaofeng Zhang,Xiaodi Ren,Lingyun Zhu,Shan Gao,Xiaowen Zhan
The poor anode/electrolyte compatibility and dendrite growth have discouraged the development of solid-state sodium-metal batteries (SSSMBs). Here, a self-formed interphase with a unique Fe valence gradient is designed to stabilize the anode interface of Na 3 Zr 2 Si 2 PO 12 solid electrolyte. This interphase consists of a Fe- and NaF-containing outer layer near the Na anode and a Fe 2+ /Fe 3+ -rich inner layer, which are in situ formed upon contacting Na with a sodiophilic α-Fe 2 O 3-x F x interlayer specially coated on Na 3 Zr 2 Si 2 PO 12 . The NaF and Fe prevents continuous reduction reactions and homogenize the electric filed, while the iron oxide gradient layer offers buffering Na storage during plating, further suppressing dendrite growth. Benefiting from the dynamically stable, low-impedance and dendrite-free interface, the symmetric cells achieve a 20-fold reduction in interfacial resistance and a fourfold enhancement in critical current density (CCD) at 25 °C, and powered a high CCD of 1.9 mA cm -2 and a 1000-h cycle life at 1 mA cm -2 at 80 °C. The corresponding SSSMBs based on Na 3 V 2 (PO 4 ) 3 cathodes deliver a capacity retention rate of 96% over 120 cycles at 1 C. This robust interface design supports one of the best electrochemical performances ever reported and offers a comprehensive solution to stabilize the Na 3 Zr 2 Si 2 PO 12 /Na interface toward practical SSSMBs.
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ELECTROCHIMICA ACTA
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2023
·
IF 6.6
Yanqing Fu,Dongdong Zhang,Pan Li,Yi Han,Juan You,Qiliang Wei,Weiyou Yang
The development of efficient non-precious metal electrocatalysts is essential for oxygen evolution reaction (OER) for water splitting. Among them, amorphous bimetallic NiFe-based compounds are recognized as one of the excellent candidates for efficient OER. Herein, the Ni-Fe-Se film is rationally designed via facile one-step electrodeposition with tailored active sites and thicknesses. Accordingly, the optimized sample, with an increased Fe-incorporation level and a thickness of ∼50 nm, shows a low overpotential of ∼290 mV at a current density of 40 mA cm −2 and long-term durability in 1 M KOH solution, representing its overall excellent OER performance. Furthermore, operando Raman and ex-situ XPS are used to identify the active sites for OER. This work provides some new insights into exploring earth-abundant free-standing catalysts for OER toward overall water-splitting applications.
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Catalysts
·
2023
·Vol. 13
·期 3
·619
·
IF 3.9
Chen Yang,Xuefeng Hu,Yaxing Bai,Beichuan Cai,Yujie Li
In this study, a simple and low-energy synthesis scheme of Fe single-atom anchored carbon nitride was reported to improve the photocatalytic performance of g-C3N4. Synthesized Fe single-atom doped graphite carbon nitride (Fe-SACs/g-C3N4) showed high activity and stability for the degradation of 2-mercaptobenzothiazole (MBT); under visible light irradiation, 99% of MBT could be degraded within 35 min, and the degradation ability basically did not decline after five cycles, mainly due to the synergistic effect of the Fe single atoms and carbon nitride. The results of X-ray absorption fine structure (EXAFS), X-ray photoelectron spectroscopy (XPS), and density functional theory calculations show that the single-atom Fe forms Fe-N4coordination with pyridine nitrogen to generate a new electron transfer channel, which can significantly improve the in-plane separation and transfer of carriers, finally enhancing the generation of superoxide radicals. This is confirmed by time-resolved photoluminescence, photoelectron chemistry, and electron spin resonance measurements. The main intermediates of MBT degradation were determined using a liquid chromatograph–mass spectrometer (LC-MS), and a possible photocatalytic mechanism based on the quenching experiment and electron paramagnetic resonance (EPR) test was proposed. A deep understanding of the contribution of Fe single-atom sites with clear local coordination structures will help to design effective catalysts for photocatalytic performance.Keywords:graphitic carbon nitride;single-atom;NaBH4reduction;photocatalytic degradation
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Zhaoyi Yang,Xiaofang Yang,Guangyu An,Dongsheng Wang
Optimization of Fe-based heterogeneous catalyst for enhancing PMS activation was studies by an electronic structure regulation strategy. The single atom and nano-particle Fe-catalysts were then modified by P-doping on carbon support and tested for BPA degradation. Catalysts with P-doping led to 100 % BPA degradation in 30 min, much better than single atom and nano-particle control groups (56 % and 61 %). Experimental and DFT results revealed that P-doping increased the electron density of Fe and induced the transformation of Fe 3d electron spin state from low spin to medium spin, then the Fe 3d orbitals with high energy could better overlap with O 2p orbitals of PMS, promoting the electron transfer process from Fe to PMS and generation of hydroxyl radical. This work provides a deep understanding of spin state modulation for designing high-performance PMS activation catalysts.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 12
·6191-6197
·
IF 11.9
Hongzhou Yang,He Huang,Qing Wang,Lu Shang,Tierui Zhang,Shouguo Wang
3d transition metal single atom catalysts (SACs) (e.g. M = Fe, Co, Cu) are considered as promising catalysts for oxygen reduction reaction (ORR), among which Fe SACs display comparable performance to commercial Pt/C. However, Fe SACs still demand significant improvements in activity and stability for further industrial deployment. Herein, a Fe, Cu dual metal SAC was synthesized using a facile ligand-mediated method. Fe and Cu atoms were atomically dispersed on commercial carbon black in the form of FeN4 and CuN4 sites. Owing to the interactions between the adjacent Fe and Cu atoms co-existing in a very tiny area, the as-synthesized Fe, Cu dual metal SAC exhibited excellent ORR performance with a high half-wave potential of 0.926 V and good stability in 0.1 M KOH, which are significantly higher than that of the Fe-SAC or Cu-SAC control samples. Density function theory calculations showed that the Cu single atom can act as an electron donator enriching the electron density of Fe sites, thus endowing the Fe sites with optimized adsorption/desorption energy for ORR intermediates and thereby facilitating the ORR activity of FeCu-SAC. Moreover, a study on three typical commercial carbon substrates indicated that carbon support with high surface areas and hierarchical pore structure was beneficial for ORR. The excellent ORR activity and durability of FeCu-SAC enabled the constructed Zn–air battery to have a high power density of 201.4 mW cm−2 and high specific energy of 827.68 W h kg−1.
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CHEMOSPHERE
·
2019
·
IF 5.108
Ruijie Xie,Gaoyuan Liu,Dingping Liu,Shimin Liang,Dongxue Lei,Hanying Dong,Haibao Huang,Dennis Y.C. Leung
The traditional treatment processes for volatile organic compounds (VOCs) removal generally suffered several disadvantages, such as secondary air-pollutants. To overcome these issues, wet scrubber coupled with heterogeneous UV/Fenton was developed for gaseous VOCs (i.e. toluene) removal. ZSM-5 supported iron oxide (Fe/ZSM-5) was prepared as a multifunctional catalyst for activation of H 2 O 2 and enhancement of gas-liquid mass transfer. Toluene was removed efficiently by this coupled process with the removal efficiency of 85% during 120 min. Many intermediates were detected in the solution by GC-MS while no intermediates were observed in the outlet gas, suggesting that wet scrubber coupled with heterogeneous UV/Fenton could significantly reduce secondary air pollutants . The possible mechanism of toluene oxidation was proposed including the physical adsorption by Fe/ZSM-5 and OH oxidation. This study provides an environmentally benign and highly efficient chemical scrubbing process for gaseous VOCs removal.
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WATER RESEARCH
·
2019
·
IF 7.913
Shuhui Sun,Shu Wang,Yuxuan Ye,Bingcai Pan
Considerable amount of phosphorous is present as organic phosphonates (usually in the form of metal complexes, e.g., Ca(II)-phosphonate) in domestic and industrial effluents , which cannot be effectively removed by traditional processes for phosphate. Herein, we employed a proprietary process, i.e., Fe(III) displacement/UV irradiation/co-precipitation (denoted Fe(III)/UV/NaOH), to enable an efficient removal of Ca(II)-phosphonate complexes from water. The combined process includes three basic steps, i.e., Fe(III) replacement with the complexed Ca(II) to form Fe(III)-phosphonate of high photo-reactivity, UV-mediated degradation of Fe(III)-phosphonate to form phosphate and other intermediates, and the final phosphorous removal via co-precipitation at pH = 6. The operational conditions for the combined process to remove a typical phosphonate Ca(II)-NTMP (nitrilotrismethylenephosphonate) are optimized, where ∼60% NTMP is transformed to phosphate with the total phosphorous reduction from 1.81 mg/L to 0.17 mg/L. Under UV irradiation, the cleavage of NTMP is identified at the C-N and C-P bonds to form the intermediate products and phosphate in sequence. Also, the combined process is employed for treatment of two authentic effluents before and after activated sludge treatment, resulting in the phosphorous drop from 4.3 mg/L to 0.23 mg/L and from 0.90 mg/L to 0.14 mg/L respectively, which is much superior to other processes including Fenton/co-precipitation. In general, the combined process exhibits great potential for efficient removal of phosphonates from contaminated waters .
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