Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 27
·16863-16876
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IF 10.7
Katam Srinivas,Hesheng Yu,Zhuo Chen,Anran Chen,Ming-qiang Zhu,Yuanfu Chen,Chengtao Yang
The urgent demand for stable and highly efficient bifunctional electrocatalysts for the oxygen reduction/evolution reactions (ORR/OER) is pivotal in advancing energy conversion and storage technologies. Herein, we introduce a metal–organic framework (MOF)-derived bifunctional electrocatalyst Fe3Co-NC@900, featuring synergistically coupled dual single-atom sites (Fe/Co–Nx) and core–shell Co3Fe7@C nanoparticles. Leveraging the synergistic interactions of Fe–Nx sites with associated Co–Nx sites and core–shell nanoparticles within the MOF-derived nitrogen-doped mesoporous sheets and nanotubes, Fe3Co-NC@900 demonstrates outstanding ORR and OER performance, outpacing the Fe-NC@900 catalyst fabricated without Co incorporation. Specifically, it demonstrates superior ORR performance with a higher half-wave potential (E1/2) of 0.88 V and a small Tafel slope of 62.1 mV dec−1, surpassing the Pt/C benchmark (E1/2 of 0.82 V) and Fe-NC@900 (E1/2 of 0.788 V). Additionally, it demonstrates noteworthy OER performance, requiring a 1.572 V overpotential at 10 mA cm−2 current density, resulting in a significant bifunctional activity with a potential gap (ΔE) of 0.692 V, surpassing the Pt/C + Ir/C combination (ΔE = 0.748 V). Moreover, serving as a bifunctional air electrode, Fe3Co-NC@900 exhibits excellent performance in lab-made Zn–air batteries, with outstanding open circuit voltage, specific capacity, and cycling stability (>650 cycles), outpacing the Pt/C + Ir/C-based battery.
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高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Jiapeng Wang,Xinpeng Chen,Hua-Bin Yuan,Lili Xing,Desheng Sha,Aijing Li,Guoqiang Chen,Tieling Xing
Metal-organic frameworks (MOFs) find wide-ranging applications owing to their adjustable structures, diverse compositions, and large specific surface area. In this work, MOFs materials were grown in situ on carbon cloth, yielding self-supported electrodes V O -(Fe,Co) 3 O 4 @CC rich in oxygen vacancies through a simple high-temperature annealing treatment utilizing NaBH 4 as an etchant. Thus the resulting self-supported electrode V O -(Fe,Co) 3 O 4 @CC exhibited excellent oxygen evolution reaction (OER) performance, achieving an overpotential of merely 288 mV at 10 mA cm −2 , along with a low Tafel slope of 31.39 mV dec -1 , and demonstrating robust long-term activity and stability. In addition, a liquid zinc-air battery was assembled utilizing the prepared V O -(Fe,Co) 3 O 4 @CC as an air cathode, achieving a high open-circuit voltage of 1.46 V and a high peak power density of 89.06 mW cm −2 , and it maintained excellent cycling stability during cyclic charging and discharging (with a current density of 2 mA cm −2 ) over a 32 h period. Meanwhile, the self-supported electrode V O -(Fe,Co) 3 O 4 @CC served as an air cathode for assembling an all-solid-state flexible zinc-air battery (ZAB), demonstrating a high peak power density (38.21 mW cm −2 ) and exhibiting favorable cycling stability. This experiment offers insights into the potential application of MOF-derived electrocatalysts in water decomposition and zinc-air batteries.
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高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 8
·087501
·
IF 4.316
Shiying Zhou,Peng Zhao,Jilin Zheng,Sha Chen,Mei Yang,Danqun Huo,Changjun Hou
Flexible electrodes play an increasingly important role in the development of portable and wearable electronics. Herein, a novel flexible and self-supporting electrode supported on active electrocatalyst (Au/Fe–Co@C–Nx/GO/CC) has been prepared for in situ detection of extracellular H2O2. The Fe, N co-doping of Fe–Co@C–Nx with abundant active sites promotes electron transfer efficiency, and Fe–Co@C–Nx nano-arrays with a unique spatial structure are beneficial for the deposition of Au nanoparticles (AuNPs). Graphene oxide (GO) serves as a chemical bridge to ensure that the nanomaterials grow more uniformly and firmly on the carbon cloth. Meanwhile, the flexible carbon cloth possesses stable mechanical and electrochemical properties. Based on these unique superiorities, this flexible electrode exhibits excellent sensing performance toward H2O2 with high selectivity and sensitivity, low LOD (0.56 μM), and wide linear range (from 5 to 21195 μM). Most importantly, the prepared electrode can adhere to cells for in situ and sensitive determination of H2O2 released from cells. Compared to detecting H2O2 in cell suspensions, in situ detection can capture the signal molecules more sensitively and effectively, avoiding the diffusion of H2O2 from the solution to the electrode surface. This flexible electrode has great potential in development of molecular detection and portable electronics.
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RSC Advances
·
2015
·Vol. 5
·期 60
·48946-48953
·
IF 3.84
Tingting Yu,Lifen Liu,Qiao Yang,Jing Song,Fenglin Yang
Using the flat module membrane electrodes based on polyester filter modified with polyaniline (PANI)–phytic acid (PA), a new type of membrane bio-reactor (MBR) system is developed for both bio-electrochemical electricity generation and effluent filtration. A specifically prepared carbon foam–Fe–Co catalyst was coated on the conductive, filterable cathode membrane which makes it catalytic for enhancing cathodic oxygen reduction reaction and electricity generation. The cell voltage (with carbon foam–Fe–Co, 0.5–0.4 V) is superior to control test 1 (without any catalyst, 0.2 V), moreover, it is even better than control test 2 (with Pt–C catalyst, 0.5–0.3 V). The corresponding maximum power density of carbon foam–Fe–Co is 38.5 and 2.4 times higher than control test 1 and 2, respectively. More importantly, the base electrode materials and catalyst were both low-cost. The overall removal efficiency of COD and NH4+–N are satisfactory, at 95% ± 2.5% and 85% ± 2.5%, respectively. This integrated system is easy to scale up for practical application in waste-water treatment and offers a better option in operating and coupling MBR with bio-electricity generation.
研究领域:
环境工程
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环境微生物学
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电化学工程
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水处理技术
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生物电化学系统
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高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 10
·106507
·
IF 4.386
Mengxue Huang,Ruimin Ding,Jie Yang,Wenwen Shi,Shufang Shi,Lifang Chen,Shanshan Liu,Xi Yin
Platinum group metal-free catalysts based on transition metal and nitrogen co-doped carbon materials are gaining attention for their applications in electrocatalysis. Nitrogen-coordinated metal sites (MNx) have been identified as the main active sites in PGM-free catalysts. Current synthetic approaches rely on the high-temperature treatment to introduce targeted electroactive MNx sites into the carbon matrix. In this study, we demonstrated the formation of MNx sites on Ni- and N-co-doped carbon templates via the solution-phase coordination with target metal ions, including Fe2+, Fe3+, and/ Co2+. The formation of MNx sites was confirmed via a combined approach of various physical characterization techniques, elemental analysis, and electrochemical analysis. The results indicate that the metal-vacancy-Nx sites in the template can coordinate with target ions to form electrochemically active MNx sites. By varying heat-treatment temperature, the amount of FeNx sites formed via coordination with Fe2+ ion can be tuned and correlated with the change of activity toward oxygen reduction reaction. The amount of MNx sites formed via solution-phase coordination with various ions followed the sequence of Co2+ > Fe2+ > Fe3+. These findings may further guide the future development of MNx-C electrocatalysts through this solution-phase coordination approach.
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高影响因子
ELECTROCHIMICA ACTA
·
2026
·
IF 5.8
Yutong Yang,Lijie Zhao,Ning Liu,Jianjiao Xin,Wanli Yang,Xinyou Zhang,Danfeng He,Fujiang Zhou,Hong Pan
La 3+ /Fe 2+ co-doping tailors U and W of CoO for bulk electronic optimization. • La 3+ -induced distortion reconstructs Lewis base sites to suppress shuttle effect. • Base sites show strong Li + adsorption and weaken S-S bonds via electron injection. • As supercapacitor cathode: 1405.6 F g −1 at 1 A g −1 , device energy 93.0 Wh kg −1 . • As Li-S sulfur host: 1161.6 mAh g −1 at 0.1 C, 62.1% retention after 100 cycles. This work develops La/Fe co-doped cobalt oxide (La/Fe-CoO) as a bifunctional electrode material to simultaneously enhance the electrochemical performance of supercapacitors and lithium-sulfur batteries, targeting the common bottlenecks of sluggish charge transport and poor surface reaction kinetics. The performance limitations of CoO arise primarily from its unfavorable electronic structure parameters: excessive Hubbard repulsion energy ( U ) and narrow band width ( W ), which severely restrict redox efficiency and electron conductivity. To address these issues, La 3+ and Fe 2+ co-doping is employed to achieve precise synergistic regulation of U and W . Fe 2+ doping constructs an extended “Co 3d -O 2p -Fe 3d ” orbital hybridization network that broadens W , optimizes charge transport pathways, and substantially improves intrinsic conductivity. Meanwhile, La 3+ reduces the effective Hubbard U through f-d orbital coupling, weakening intraorbital electron repulsion and lowering the reaction barrier. More importantly, the large ionic radius of La 3+ induces local lattice distortion, generating abundant electron-rich Lewis basic active sites on the material surface, which are distinctly different from the Lewis acidic sites commonly reported in the literature. Unlike acidic sites based on metal cations, these basic sites not only immobilize polysulfides by electrostatically adsorbing Li + ions, but also inject electrons into the S-S antibonding orbitals, exerting a redox catalytic effect that promotes S-S bond cleavage and accelerates polysulfide conversion kinetics, thereby effectively suppressing the shuttle effect in lithium-sulfur batteries. This work, through the synergistic design of bulk electronic structure ( U / W ) modulation and surface basic site reconstruction, offers a feasible strategy for developing high-performance bifunctional electrode materials for energy storage applications. Download: Download high-res image (412KB) Download: Download full-size image
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Lei Yang,Zifei Wei,Zihan Guo,Mengfang Chen,Jingchun Yan,Linbo Qian,Lu Han,Jing Li,Mingyue Gu
CoFe 2 O 4 /hydrochar composites (FeCo@HC) were synthesized via a facile one-step hydrothermal method and utilized to activate peroxymonosulfate (PMS) for simultaneous degradation of monochlorobenzene (MCB) and p-chloroaniline (PCA). Additionally, the effects of humic acid , Cl - , HCO 3 - , H 2 PO 4 -, HPO 4 2- and water matrices were investigated and degradation pathways of MCB and PCA were proposed. The removal efficiencies of MCB and PCA were higher in FeCo@HC140–10/PMS system obtained under hydrothermal temperature of 140 °C than FeCo@HC180–10/PMS and FeCo@HC220–10/PMS systems obtained under higher temperatures. Radical species (i.e., SO 4 • - , •OH) and nonradical pathways (i.e., 1 O 2 , Fe (IV)/Co (IV) and electron transfer through surface FeCo@HC140–10/PMS* complex) co-occurred in the FeCo@HC140–10/PMS system, while radical and nonradical pathways were dominant in degrading MCB and PCA respectively. The surface functional groups (i.e., C-OH and C O) and Fe/Co redox cycles played crucial roles in the PMS activation . MCB degradation was significantly inhibited in the mixed MCB/PCA solution over that in the single MCB solution, whereas PCA degradation was slightly promoted in the mixed MCB/PCA solution. These findings are significant for the provision of a low-cost and environmentally-benign synthesis of bimetal-hydrochar composites and more detailed understanding of the related mechanisms on PMS activation for simultaneous removal of the mixed contaminants in groundwater.
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PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Wei Wen,Xiaoqiang Du,Xiaoshuang Zhang
Replacing fossil fuels by electrocatalytic water splitting for producing hydrogen and oxygen is one of the most promising ways to solve the energy crisis and environmental pollution. In this work, a series of M doped N-Ni 3 S 2 (M = Cu, Fe, Co and Ce) material was firstly synthesized and in situ grown on nickel foam substrate by a typical two-step hydrothermal synthesis method. Two probe reactions, water oxidation and urea oxidation, were selected to investigate the catalytic performance of these materials. What is noteworthy is that the Fe doped N-Ni 3 S 2 material exhibits superior water oxidation properties with requiring only 270 mV of overpotentials to drive current densities of 100 mA cm −2 , which is one of the best activities reported so far. After a long time of durability measurement, the current density of the Fe doped N-Ni 3 S 2 material will be attenuated, suggesting that the surface of the material will be in situ oxidized to oxide or hydroxide, which is the true active species. For urea oxidation, the Co doped N-Ni 3 S 2 material shows superior catalytic performance with requiring only 1.36 V potentials to drive 100 mA cm −2 current densities. Density functional theory (DFT) calculation shows that different adsorption energy of water for N-Ni 3 S 2 , N-Cu-Ni 3 S 2 , N-Fe-Ni 3 S 2 and N-Co-Ni 3 S 2 leads to the different catalytic activity. Experimental results demonstrate that the improved catalytic performance is assigned to faster electron transfer rates, exposure of abundant active center and better conductivity due to N and cation doping. This work provides new lessons for doping engineering for water splitting reactions.
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高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Chunmei Xu,Mengran Lou,Rui Liu,Taotao Lv,Yang Wang,Ruiying Wang,Hongtao Liu,Xia Kong
Metal-nitrogen-carbon (M–N–C) catalysts are promising alternatives to precious metal-based bifunctional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in Zn-air batteries (ZABs). Herein, FeCo@nitrogen doped carbon nanotube/nitrogen doped reduced graphene oxide (FeCo@NCNT/N-rGO) catalyst with unique 3D heterostructure was synthesized through one-step pyrolysis of FeCo-ZIF-8 precursor anchored on graphene oxide (FeCo-ZIF-8/GO). Benefiting from the coupling of FeCo dual-metal sites with nitrogen-doped carbon substrates, the FeCo@NCNT/N-rGO catalyst achieved extraordinary bifunctional oxygen electrocatalytic activity, exhibiting a high ORR half-wave potential (E 1/2 ) of 0.881 V (vs. RHE), which was superior to the Pt/C catalyst (0.838 V), and OER overpotential of 343 mV at 10 mA cm −2 , merely inferior to RuO 2 by 33 mV. The resulting ΔE (defined as E j=10 − E 1/2 ) reaches an impressively low value of 0.69 V, highlighting its superior reversible oxygen electrocatalytic performance. Meanwhile, achieving a high-power density of 240 mW cm −2 and open circuit voltage (OCV) of 1.488 V in ZAB applications, superior to that of Pt/C + RuO 2 in ZAB (1.447 V; 143 mW cm −2 ). Flexible solid-state ZAB with FeCo@NCNT/N-rGO achieves 1.416 V OCV and 47.4 mW cm −2 power density, remaining stable even when bent 180°. This study guides design of dual-site non-precious metal bifunctional oxygen catalysts.
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高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Zizheng Zhu,Hongyan Zhang,Wen Guo,Hao Zhou,Yilin Zhou,Wenjie Liang,Maoshuai He,Wenxian Wei,Tingting Yu,Hong Zhao,Tao Yang
The highly efficient catalysts for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are of great significance for electrochemical water splitting. Direct transforming nickel foam (NF) into nickel-based catalysts attracts extensive attention because of its excellent stability and high conductivity. However, the catalytic performances of this kind of catalyst are still far from expected. Herein, we report a series of Ni oxides co-modulated by Mo, V and M ( M =Mn, Fe, Co, Cu) as efficient catalysts for water splitting, which are directly prepared through a simple NF-transformation method. Especially, a MoVNi catalyst displays a low Tafel slope of 68 mV/dec and a small overpotential of 76 mV at 10 mA/cm 2 for HER in 1.0 M KOH solution. The OER performances of MoVNi can be greatly enhanced by M introduction. For example, Fe-MoVNi only requires 374 mV to achieve 100 mA/cm 2 and shows no declination in a-20 h stability test at 100 mA/cm 2 in 1.0 M KOH media. Such performances outperform the recently reported best-performing Ni oxides catalysts in an alkaline environment. The excellent catalytic performances suggest great promise in practical applications.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ying Fang,Qianwen Liu,Yang Song,Feiyue Jia,Ying Yang,Haipu Li
Dissolved organic matter (DOM) extensively exists in high-arsenic groundwater with relatively high concentration, which could not only compete with arsenic for adsorption sites, but also depress As(III) oxidation in persulfate-based advanced processes (PS-AOPs) through scavenging free radicals (SO 4 • − and •OH). In order to effectively avoid the negative effect of DOM , an Fe/Co bimetallic metal–organic framework (Fe/Co MOF)-coupled peroxymonosulfate (Fe/Co MOF-PMS) system was rationally constructed for non-radical-dominated As(III) oxidation and chemisorption-driven As(V) adsorption. Results showed that the Fe/Co MOF-PMS system did realize anti-interference As(III) immobilization in DOM-rich high-arsenic groundwater, which was evidenced by no difference in As(III) immobilization efficiencies in the absence and presence of 20 mg/L humic acid (HA). During the oxidation process, 1 O 2 dominated As(III) oxidation while O 2 • − dominated HA oxidation, and the presence of HA significantly promoted the generation of 1 O 2 besides SO 4 • − and •OH. During the adsorption process, chemical adsorption mainly drove As(V) adsorption such as forming M-O-As (M = Fe, Co) bond, while physical adsorption forces played a major role in HA adsorption, such as π-π interaction, hydrogen bonding, and electrostatic attraction. The synergism of oxidation and adsorption processes made the anti-interference As(III) immobilization in DOM-rich high-arsenic groundwater in Fe/Co MOF-PMS system come true. This work is believed to shed light on the highly efficient purification of DOM-rich high-arsenic groundwater.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 18
·8739-8751
·
IF 3.925
Quansheng Wu,Songhua Zhou,Chengbing Fu,Jiesong Zhang,Bo Chen,Hongyan Pan,Qian Lin
For the mono-metal Pd based catalysts, the O–O bond in O2 and H2O2 is easily dissociated due to the higher energy sites of Pd, which decreases the selectivity and productivity of H2O2. To address this issue, non-noble metals M (M = Sn, Fe, Co, Ni) were doped into palladium precursors to create a series of yolk–shell structure bimetallic catalysts Pd–M@HCS (H = hollow; C = carbon; S = sphere) with Pd–M as the core and porous carbon as the shell. The results indicated that the catalyst Pd–M@HCS doped with Sn, Fe, Co, and Ni has a weak dissociation ability for O2, and both the adsorption and dissociation ability for H2 are improved. Of these catalysts, the catalyst Pd–Sn@HCS gives the best performance, which is benefited by the suitable Pd–Sn nanoparticle size and the best Pd2+/Pd0 ratio. The influence of the nPd/nSn ratio in the Pd–Sn@HCS system on catalyst performance was further explored, and the findings revealed that Pd–Sn@HCS had the best catalytic activity and stability when the nPd/nSn ratio was 2. The catalyst's H2 conversion, H2O2 selectivity, and productivity were 35%, 97%, and 3961 mmol gPd−1 h−1, respectively. After 10 cycles, the H2O2 productivity of this catalyst remained at 92.1%, which was greater than the H2O2 productivity of the typical Pd-based catalyst Pd/C, which stayed at 37% under the same conditions.
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