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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Catalysts
·
2023
·Vol. 13
·期 3
·619
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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
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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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INORGANIC CHEMISTRY COMMUNICATIONS
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2023
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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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Energies
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2023
·Vol. 16
·期 9
·3684
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IF 3.2
Ruimin Zhang,Ke Wang,Peng Wang,Yan He,Zhiming Liu
Single-atom catalysts (SACs) within carbon matrix became one of the most promising alternatives to noble metal-based catalysts for oxygen reduction reaction (ORR). Although SACs have significant benefits in reducing the total catalyst cost, it also has the disadvantages of weak interaction between atoms and poor stability. Hence, there is still much room for improvement for the catalyst activity. In response, we designed a Fe-Co-Pt ternary metal single atom catalyst anchored on covalent organic framework (COF)-derived N-doped carbon nanospheres (Pt, Fe, Co/N-C). Due to effective charge transfer between Pt single atom and neighboring Fe-Co components, an intense electron interaction can be established within the Pt, Fe, Co/N-C catalyst. This is beneficial for enhancing charge transfer efficiency, modulating d electronic structure of Pt center and weakening oxygen intermediate adsorption, thus distinctly accelerating ORR catalytic kinetics. As expected, the half-wave potential of Pt, Fe, Co/N-C was 0.845 V, much higher than those of commercial 20 wt% Pt/C (0.835 V), Pt/N-C (0.79 V) and Fe, Co/N-C (0.81 V) counterparts. Moreover, the Pt, Fe, Co/N-C catalyst demonstrated much-improved cycling stability and methanol tolerance.Keywords:oxygen reduction reaction;electrocatalysts;single atom;ternary metal;kinetics
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ENVIRONMENTAL TECHNOLOGY
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2023
·
IF 2.8
Yi Ding,Min Zhang,Sijie Zhou,Linbei Xie,Ao Li,Ping Wang
Ferrous iron (Fe(II)) reacts with peroxymonosulphate (PMS) to form active oxidants that can degrade refractory organic pollutants. However, the conversion rate of Fe(III) to Fe(II) is slow, which limits its actual application. In the study, the effect of fulvic acid (FA) on the degradation of dimethyl phthalate (DMP) by Fe(II)/PMS was investigated. Moreover, the degradation process of DMP was predicted by the preliminary identification of active free radicals and intermediates. As expected, FA gave rise to a higher concentration of Fe(II) than that in Fe(II)/PMS to enhance the removal of DMP in Fe(II)/PMS system. The precipitate, involved in FA and iron, was an important composite to promote the degradation of DMP in the system. Also, the response surface methodology (RSM) was applied to model and optimize the degradation conditions of DMP. The highest removal efficiency (85.70%) was obtained at pH = 3.86, [PMS] = 0.96 mM, [FA] = 11.44 mg/L and [DMP] = 5 µM. The results of free radical quenching experiments and EPR showed that •OH and SO4•− were the main active radicals in this system. The degradation intermediates of DMP were monomethyl phthalate (MMP), phthalic acid and benzoic acid. Discoveries of this study had raised the current understanding of the application of FA keeping the cycles of Fe(II)/Fe(III) for peroxymonosulphate activation, which could afford valuable information for the degradation of organic pollutants by FA/Fe(II)/PMS.
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PubMed
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
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2023
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IF 4.6
Jingjuan Lai,Fengyu Guo,Li Wang,Chunxia Zhao,Dong Xiang,Hui Li,Bin Wang,Peng An,Zhenyu Li,Hongwei Zhou,Yuanpeng Wu
With the acceleration of the industrial process, oil-water separation is an urgent problem for oil spill accidents and wastewater treatments. Exploiting superhydrophobic materials applied in harsh environments and remote drives remains a significant challenge in solving oil moisture problems. An alternative strategy to solve this problem has been demonstrated by decorating poly lauryl methacrylate (LMA) on Fe foam via the solution polymerization method. The as-prepared Fe foam possesses good superhydrophobicity (>150°) under broad pH (1 < pH < 12) and a wide temperature range (−55°C-180 °C). Furthermore, outstanding separation efficiency (>99.1%), high cycle stability (>50 times), and high oil flux (63.7–114.6 kL m −2 h −1 ) against diverse oil/water mixtures can be realized under gravity. Interestingly, oil harvesting capacity above or beneath the water can be realized by remote magnetic driving as well.
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ELECTROCHIMICA ACTA
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2023
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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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Journal of Materials Research and Technology-JMR&T
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2022
·
IF 6.267
Jingwu Zheng,Siyuan Wang,Shuan Zhang,Wei Cai,Liang Qiao,Haibo Chen,Yao Ying,Wangchang Li,Jing Yu,Shenglei Che
In this paper, a corrosion-resistant glutamic acid (Glu)-Cu-Nano-Al 2 O 3 composite coating with both hydrophobicity and self-healing characteristics was electrodeposited on the sintered Nd-Fe-B surface. The influence of the amount of Nano-Al 2 O 3 added in the acidic Cu 2+ -glutamate (Glu 2− ) solution on the performance of the composite coating was studied, the results show that Nano-Al 2 O 3 inclusion can make the surface of the composite coating appear papillary particles and make the composite coating hydrophobic. By analyzing the products of the composite coating after corrosion in 3.5% NaCl solution, it is shown that the codeposition copper dihydroglutamate (CuGlu 2 H 2 ) and Glu particles in the composite coating are released and dissolved in the solution with pH = 6.5 after copper corrosion, and then complexed with Cu 2+ produced by corrosion to form an insoluble copper glutamate (CuGlu) passive film, which was deposited on the corroded coating to achieve self-repairing function and prevent further corrosion. The hydrophobicity and self-repairing function of the composite coating ensure that the sintered Nd-Fe-B has excellent corrosion resistance.
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JOURNAL OF RARE EARTHS
·
2023
·
IF 4.9
Bolang Li,Fei Wang,Kai Li,Ping Ning,Min Chen,Changbin Zhang
The chemical transformation of CO 2 produces carbon compounds that can be used as precursors for the production of chemicals and fuels. Here, we investigated the activity and selectivity of the transition metals (Fe, Co, and Ni) supported on CeO 2 catalyst for CO 2 hydrogenation at atmospheric pressure. We found that Ni/CeO 2 shows the highest CO 2 conversion compared with Fe/CeO 2 and Co/CeO 2 . Besides, Co/CeO 2 and Ni/CeO 2 exhibit nearly 100% CH 4 selectivity while Fe/CeO 2 inclines to produce CO. The characterization results show that the metal-support interaction order is Fe/CeO 2 > Co/CeO 2 > Ni/CeO 2 , the weak metal-support interaction over Ni/CeO 2 benefits the activation of H 2 and then promotes the activity of CO 2 hydrogenation. Additionally, in situ DRIFTS results demonstrate that monodentate formate species rather than bidentate formate are the active intermediates. The main route of CO 2 hydrogenation to CH 4 is that CO 2 is firstly transformed to m-HCOO∗ and then direct hydrogenation of the m-HCOO∗ to CH 4 . This study provides insights into the understanding of the mechanisms of CO 2 hydrogenation on CeO 2 based catalysts.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Zhuoyue Liu,Ke Wang,Danyang Li,Zhenxin Wang,Shengjiong Yang,Heliang Pang,Gen Wang,Dahu Ding,Delu Miao
Mesoporous carbon materials are promising catalysts for peroxydisulfate (PDS) activation for degrading aqueous organic pollutants but limited by the intrinsic inertness. Herein, co-doping of iron and nitrogen into the mesoporous carbon framework was performed via thermal conversion of metal-polyphenol coordination polymers (Fe-TA) to synthesize Fe/N co-doped mesoporous carbon for efficient PDS activation. Owing to the large surface area, high graphitization degree and defective configurations, the Fe/N co-doped mesoporous carbon (Fe/N-MCs) exhibited superior catalytic performance toward the degradation of organic pollutants . Electron paramagnetic resonance tests, chemical quenching experiments, electrochemical analysis and spectra measurements revealed that the degradation of organic pollutants over the Fe/N-MCs followed a nonradical oxidation pathway based on electron transfer process. Graphite nitrogen and hydroxyl (C-OH) groups on the defective edges of Fe/N-MCs were proved to be possible active sites for PDS activation. PDS catalyzed by the Fe/N-MCs exhibited strong anti-interference capability to surrounding inorganic ions (such as Cl – , CO 3 2– , NO 3 – and SO 4 2– ) and natural organic matters, making it a promising candidate for the degradation of organic pollutants. This work provides a new prospect for developing highly active mesoporous carbon materials via heteroatom doping for PDS activation for wastewater decontamination .
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Shujuan Lv,Ying Deng,Qian Liu,Ziqi Fu,Xiaobin Liu,Minghui Wang,Zhenyu Xiao,Bin Li,Lei Wang
The hollow materials with open structure can accelerate the mass transfer and bubble release rate, which have attracted tremendous attention for electrocatalytic water splitting. In this work, a unique tri-metal phosphide open nanotube structure [FeCoNiP@carbon quantum dots, FCNP@CQDs] is firstly fabricated by a selected etching and phosphating process with a MIL-88A@CQDs (MIL stands for Material of Institute Lavoisier) as the precursor. Benefiting from their open structure, FCNP@CQDs exhibit excellent catalytic performance. In alkaline seawater solution, a low overpotential of 268 mV is required to reach 20 mA cm −2 current density for oxygen evolution reaction, while the η 20 of hydrogen evolution reaction is 150 mV. The FCNP@CQDs//FCNP@CQDs electrolyzer requires a voltage of 1.61 V to reach 10 mA cm −2 . The integrated strategy of CQDs-doping and construction of hollow open structures may open a new and relatively unexplored path for fabricating high-performance seawater splitting catalysis.
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