INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
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IF 5.816
Dongting Wu,Aiqun Kong,Wei Li,Yan Fu,Jinli Zhang
Bimetallic Ni–Fe phosphide electrocatalysts were in-situ synthesized through direct phosphorization of metal salts on carbon cloth (CC). The Fe dopant remarkably enhances the OER performance of Ni 2 P in alkaline medium through the electronic structure modulation of Ni. The (Fe 0.5 Ni 0.5 ) 2 P/CC electrode, composed of uniform films coated on carbon fibers, delivers a low overpotential of 260 mV with a small Tafel slope of 45 mV·dec −1 at the current density of 100 mA cm −2 , outperforming most reported non-noble electrocatalysts and commercial RuO 2 electrocatalyst. The (Fe 0.5 Ni 0.5 ) 2 P/CC also displays superior electrochemical stability at high current density . An appropriate Fe dopant level facilitates the in-situ transformation of Ni–Fe phosphides into active NiFeOOH during alkaline OER. This work simplifies the synthesis procedure of metal phosphides.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
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IF 5.816
Ruihui Gan,Yali Wang,Wenjun Ma,Mahmut Dirican,Sa Zhao,Yan Song,Xiangwu Zhang,Chang Ma,Jingli Shi
It is highly desirable to develop high-efficiency non-precious electrocatalysts toward oxygen reduction reaction (ORR). In this work, Fe 2 O 3 -encapsulated and Fe-Nx-containing porous carbon spheres (Fe 2 O 3 /N-MCCS) with unique multi-cage structures and high specific surface area (1360 m 2 g −1 ) are fabricated. The unique porous structure of Fe 2 O 3 /N-MCCS ensures fast transportation of oxygen during ORR. The combined effect of Fe 2 O 3 nanoparticles and Fe-Nx configurations endows Fe 2 O 3 /N-MCCS (E 1/2 = 0.837 V vs. RHE) with superior ORR activity and methanol tolerance to Pt/C. And, Fe 2 O 3 /N-MCCS exhibits better stability than nitrogen-modified carbon. The characterization results of Fe 2 O 3 /N-MCCS after long-term test reveals its excellent structural stability. Impressively, zinc-air battery based on Fe 2 O 3 /N-MCCS showed a peak power density of 132.4 mW cm −2 and a specific capacity of 797 mAh g −1 , respectively.
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ChemCatChem
·
2021
·Vol. 13
·期 11
·2683-2690
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IF 5.686
Xinxin Jin,Yan Xie,Junhong Fu,Chaoyue Zhao,Yinghao Xu,Yang Lv,Bingsen Zhang,Keju Sun,Rui Si,Jiahui Huang
Graphical ORR : We fabricated a FeSA/HNPC electrocatalyst with well atomically dispersed FeN 4 species. DFT calculations uncovered that the single-atomic FeN 4 sites within FeSA/HNPC electrocatalyst present in the configurations of pyrrole-N 4 −Fe are more favorable than those of pyridine-N 4 −Fe for boosting ORR performances. Atomically dispersed Fe−N−C electrocatalysts have displayed excellent catalytic performances towards the oxygen reduction reaction (ORR), while the identification of the genuine active sites remains a challenge. Herein, we report a Fe−N−C electrocatalyst of FeSA/HNPC featuring single-atomic FeN 4 sites on hierarchically N-doped porous carbon (HNPC), which shows a very competitive ORR activity in alkaline solution even at a low electrocatalyst loading of 0.2 mg cm −2 on the working electrode. A comparison of energy barriers in ORR reveals that the single-atomic FeN 4 active sites in FeSA/HNPC existing in the form of pyrrole-N 4 −Fe is more favorable than that of pyridine-N 4 −Fe for the enhanced ORR activity. Understanding the nature of FeN 4 active sites will greatly benefit the design of Fe−N−C electrocatalysts with highly effective ORR performances.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Jianan Yu,Zhiliang Zhu,Hua Zhang,Yanling Qiu,Daqiang Yin
Fenton-like catalysis has received much attention as the promising technology for organic pollutant degradation, whereas it suffers from low atomic utilization, poor catalysts durability and difficult after-treatment to hamper the catalytic oxidation activity. Herein, a Fe– and nitrogen-codoped carbon (Fe–N–C) originated from nanocellulose-based hydrochar, nitrogen source, and iron salt precursor was developed for improved PMS activation and identification of exclusive role of each species. The catalyst formed with interconnected bamboo-shaped 3D tubular structures and high Fe-doping level (up to ~9.0 wt%) not only realized excellent efficiencies in oxidative degradation of various aromatic pollutants, but was also endowed with high durability and stability toward PMS activation. Compared with that of the control catalysts only comprising either C–N network or supported Fe nanoparticles (Fe–C) with Fe IV –oxo complex sites, the co-existent active sites of Fe–N configuration and atomic Fe cluster in Fe–N–C could simultaneously improve the graphitization degree, and act as a “support” for constructing the stable structure. It is likely that the coordinated Fe–N formed with annealing process is devoted to decompose PMS by radical generation for pollutants degradation via a radical oxidation process; while the enhanced C–N bonded with graphitic N contribute to produce 1 O 2 through the nonradical processes interacted with PMS. This Fe–N–C/PMS-coupled process provided a designed strategy to construct the highly active and stable metal-nitrogen-codoped hydrothermal carbons, and deepened insights on structure-activity-stability relationship for persulfate-based environmental remediation.
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高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
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2021
·Vol. 328
·期 3
·1019-1032
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IF 1.371
Wang Yugang,Zhang Weimin,Chen Jiahong,Guo Yadan
A new type of Ca/Fe-phosphate composite CFP(CN) was prepared by a sol–gel method. The effects of pH, reaction time, initial uranium concentration, reaction temperature, and Mn(II) selective adsorption were investigated by static batch experiments. The adsorption process of CFP(CN) on U(VI) was in line with the quasi-second-order kinetic model and the Langmuir adsorption isotherm model. The results of thermodynamic analysis show that the adsorption of U(VI) by CFP(CN) is a spontaneous process with heat absorption and entropy increase. The adsorption mechanism of U(VI) on CFP(CN) was investigated by SEM, XRD and FT-IR.
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CHINESE CHEMICAL LETTERS
·
2021
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IF 6.779
Min Zhang,Bolong Yang,Ting Yang,Yahui Yang,Zhonghua Xiang
Unremitting and intensive researches about efficient non-precious metal electrocatalysts are necessary for large-scale commercial applications of fuel cells, while iron and nitrogen co-doped carbon (Fe-N-C) materials has become one of the most promising electrocatalysts to replace Pt-based noble metal catalysts . However, the traditional Fe-doped ZIF with rhomb dodecahedron morphology limits the exposure of active sites and the utilization of atoms, even affecting the performance of the catalyst. Herein, a Fe/N co-doped catalyst with a flower-like morphology was prepared using ferric citrate source along with secondary NH 3 heat treatment. The optimal catalyst (termed as 4Fe citrate -N-C-3) showed distinguished oxygen reduction reaction (ORR) activity with a half-wave potential of 0.8 and 0.9 V ( vs . RHE) in acid and alkaline media, respectively. In addition, 4Fe citrate -N-C-3 maintained more than 80% of original activity even after 50,000 s which is superior to the benchmark Pt/C. The strategy of controlling morphology and composition is meaningful for the optimization of non-precious metal electrocatalysts for ORR in fuel cells or metal-air batteries .
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高影响因子
ENVIRONMENTAL RESEARCH
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2021
·
IF 6.498
Xiang Liang,Wenhui Feng,Dong Liang,Yan Xu,Xiaoqing Qiu
Hydroxyl/amino and Fe(III) co-grafted graphite carbon nitride (CN) is fabricated via alkaline hydrothermal treatment and followed by an impregnation adsorption process. In this unique fabrication, hydroxyl and amino groups enriched on the surface play a vital role in improving the adsorption capacity for volatile organic compounds (VOCs), while the grafted amorphous Fe(III) clusters could dominantly regulate the path of molecular oxygen activation via photo-Fenton reaction, and change the selectivity of intermediate reactive oxygen species (ROS) with the assistant of the rich surficial hydroxyl groups. Meanwhile, both the grafted functional groups and Fe(III) clusters can serve as photogenerated charge acceptors for collaboratively accelerating carriers' separation. Besides, the Fe(III)-mediated interfacial charge transfer effect (IFCT) also could extend visible light absorption and boost carriers’ generation. Benefiting from the virtues of the complementary and synergy of the grafted hydroxyl/amino and Fe(III), the dual-functionalized CN is qualified as an efficient photocatalyst for removal of VOCs, which exhibits 22 and 18 times isopropanol (IPA) adsorption capacity and CO 2 production than of pristine CN during photocatalytic IPA removal, respectively. Moreover, this work provides a new strategy of surficial group-cluster bifunctionalization for systematically improving sustainable solar-to-chemical energy conversion towards VOCs mineralization.
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Tao Zhang,Xiaoying Jin,Gary Owens,Zuliang Chen
Dye-contaminated wastewater resulting from rapid industrialization and urbanization is a global problem. In this study, a ZIF-8@Fe/Ni sample was synthesized for the removal of malachite green (MG), removing more than 99% of an initial MG concentration of 50 mg L −1 within 120 min with a 318 K adsorption capacity of 151.520 mg g −1 . To understand the dye removal mechanism based on adsorption and reduction, ZIF-8@Fe/Ni was characterized by various techniques. XRD showed that the ZIF-8@Fe/Ni composite had a characteristic peak attributable to Fe/Ni around 44.8°, where the presence of Fe/Ni did not affect the structure of ZIF-8. SEM confirmed that ZIF-8@Fe/Ni was successfully prepared, while XRD and FTIR revealed that the structure of ZIF-8@Fe/Ni remained stable following the introduction of Fe/Ni. XPS showed that while Fe/Ni nanoparticles existed in ZIF-8-Fe/Ni, partial oxidation also occurred. GC–MS demonstrated the creation of two major MG degradation products, (4-aminophenyl) (phenyl) methanone and 4-aminophenol. While the overall adsorption process of MG to ZIF-8@Fe/Ni conformed to pseudo-second-order kinetics, degradation followed pseudo-first-order reduction kinetics. When applied to the remediation of wastewater, ZIF-8@Fe/Ni removed 92% of MG. Overall, this study demonstrated that ZIF-8@Fe/Ni could be a promising material for the treatment of wastewater.
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PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Libo Zhang,Lianxiang Qiu,Qingyao Zhu,Xiong Liang,Jingxiong Huang,Mengting Yang,Zhenxuan Zhang,Jiang Ma,Jun Shen
Water disinfection would result in unintended formation of halogenated disinfection by-products (DBPs) which pose potential harm to human health. In present work, Fe 78 Si 9 B 13 amorphous ribbons (Fe-Si-B AR ) showed excellent catalytic degradation performance towards an aromatic DBP, 3,5-dichlorosalicylic acid (3,5-DiClSA) by Fenton-like reaction. The catalytic degradation performances of Fe-Si-B AR , Fe 78 Si 9 B 13 crystalline ribbons (Fe-Si-B CR ) and iron powders towards 3,5-DiClSA were compared, and Fe-Si-B AR (0.0166 min −1 ) showed the fastest degradation rate. The faster surface mobility of Fe-Si-B AR , which made it easy for Fe 2+ to be oxidized by H 2 O 2 , facilitated the degradation process. High-valent iron of Fe IV could be generated which accounted for degradation of 3,5-DiClSA. The Fe-Si-B AR also showed better and better catalytic performance in 10 reuse cycles. Besides, the cytotoxicity tests indicated that the overall toxicity level of 3,5-DiClSA was declined by 88.1 % after degradation by Fe-Si-B AR . Our results showed that Fe-Si-B AR is a promising catalyst for the degradation of aromatic DBPs.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Xuqian Wang,Yi Xie,Kun Chen,Likexin Yi,Yabo Wang,Yongkui Zhang
Ferruginous rhodochrosite with high impurity is difficult to be utilized by traditional beneficiation process due to the complex characteristics. Herein, a bioleaching process driven by Acidithiobacillus ferrooxidans was proposed to recover Mn and Fe in ferruginous rhodochrosite with economic and environmental benefits. The biogenic Fe 3+ , H + and extracellular polymeric substances produced in bioleaching process significantly promoted the metal recovery and reduced the H 2 S emission. Optimal metal leaching efficiencies (95.94% of Mn and 97.54% of Fe) were achieved in bioleaching group. Furthermore, the Mn and Fe mixed leaching solutions could be directly adopted to fabricate Mn-Fe oxide based materials (MFO). When applied as catalysts for peroxymonosulfate (PMS) activation, the as-synthesized MFO performed well for sulfathiazole (STZ) degradation with a 98.66% removal efficiency in 40 min. Both radical process and non-radical process occurred in the advanced oxidation process, which induced the generation of abundant active species of ̇OH, SO 4 ̇ − and 1 O 2 . Meanwhile, charge transfer also contributed to STZ degradation. Favorably, MFO-3 exhibited good reusability in recycle study and showed adaptability towards various natural water matrixes. This research not only provided novel insights into the utilization of recalcitrant ferruginous rhodochrosite resources, but also enriched the strategy of PMS activator design for environmental remediation.
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高影响因子
CRYSTENGCOMM
·
2021
·Vol. 23
·期 13
·2538-2546
·
IF 3.545
Min Yang,Guangshe Li,Huixia Li,Junfang Ding,Yan Wang,Liping Li
Manipulating the growth behavior of nano-sized supports is proved to have extremely favorable effects for optimizing the performance of hybrid catalysts. Herein, we investigated the growth kinetics of MgFe2O4 and revealed its size-dependent behavior of Fe occupancies at octahedral and tetrahedral sites and CO oxidation catalytic activity for the first time. MgFe2O4, with particle size ranging from 8.1 nm to 190.0 nm, was prepared via a sol–gel method after post-annealing treatment at a temperature from 400 °C to 1000 °C. The growth of MgFe2O4 nanoparticles obeys the Ostwald ripening mechanism with the quantitative formula D5 = 2.08 × 1014t exp(−122.13/RT). The systematic characteristics show that the redox behavior and O2 activation of hybrid catalysts of Pt/MgFe2O4-T rely on the grain size of MgFe2O4 nanoparticles. The Pt/MgFe2O4-500 catalyst with a support size of 20.6 nm exhibits a remarkable CO oxidation performance due to its abundant chemisorbed oxygen species on the surface and enhanced metal–support interactions among all examined catalysts. Our findings offer significant insight into the size-dependent structure, redox ability and oxygen activation properties of spinel materials and can greatly impact future exploration of novel materials in heterogeneous catalysis.
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高影响因子
APPLIED ENERGY
·
2021
·
IF 9.746
Yunlei Zhao,Bo Jin,Xiao Luo,Zhiwu Liang
Many works have focused on the reactivity and valence transition of Fe-based oxygen carriers in chemical looping partial oxidation reforming process. However, the reforming performance and impacts of operating factors are unclear with the co-feeding of CaO being CO 2 carrier to realize simultaneous CO 2 capture and utilization. In this work, thermodynamic equilibrium calculation, reactivity test and material characterization are carried out to optimize the process characteristics. The impacts of feeding conditions (Fe/Al weight ratio, methane amount, Ca/Fe mole ratio and packing manner) on the reforming reactivity are obtained to reveal the interaction between CaO and Fe 2 O 3 . The gas product distribution indicates that the carbon deposition and oxidation degree is closely related to CH 4 amount. The spatial configuration between CaCO 3 and Fe 2 O 3 reforming is essential to obtain the desirable reforming products. The difference of FeO existence on the theoretical and experimental phase components illustrates that reaction degree is affected by the reduction agent amount. By comparing the methane temperature-programmed reaction of CaCO 3 , Fe 2 O 3 and their mixture, it is suggested that the existence of CaCO 3 is beneficial for accelerating iron-based methane reforming. This study provides a way to improve reaction degree and optimize process characteristic for chemical looping reforming process.
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