ACS Applied Nano Materials
·
2021
·
IF 5.097
Xiaodan Wang,Chao Wang,Fengyu Lai,Hongxia Sun,Nan Yu,Baoyou Geng
Highly efficient and stable dual-function electrocatalysts for overall water splitting are of great significance to promote the application of hydrogen energy. Constructing a bimetallic phosphide nanocomposite structure can enhance active sites and accelerate electron transfer, which is beneficial to electrocatalysis. Herein, we obtained self-supporting cobalt-iron phosphide nanosheets supported on foamed nickel through two-step hydrothermal and phosphating treatment. When the CoFe-P/NF-1 electrode material reaches 100 mA cm–2, only a HER overpotential of 180 mV is required. Moreover, the overpotential for OER is 275 mV at 200 mA cm–2. The overall water splitting electrolyzer assembled by CoFe-P/NF-1 can reach a current of 10 mA cm–2 at 1.57 V. The catalytic performance is better than the currently reported transition metal-based catalysts, and it exhibits excellent stability. This work provides a design idea of transition metal phosphide used in overall water splitting catalysis.
研究领域:
材料科学
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电化学
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能源材料
·
催化
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DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2024
·
IF 3.2
Xiaoyu Chen,Xiaoshuai Yu,Chuncheng Yang,Guoyong Wang
The oxygen evolution reaction is more challenging than the hydrogen evolution reaction in overall water splitting, not only because the four-electron reaction is more complex but also because the oxidizing environment of the anode reaction is more destructive to the electrode material. Generally, such destruction results in the formation of an oxide film that hinders the transition of electrons and subsequently decelerates the succeeding reaction. This paper proposes a transition layer for self-supporting electrodes (NiFe LDH@NiCoP/NF) in which NiCoP grows between the NF and NiFe LDH. The implementation of NiCoP as a transition layer, showcasing excellent antioxidation capability and conductivity, effectively reduced overpotentials and consequently enhanced the catalytic performance. Benefiting from this transition layer, in a 1.0 M KOH, the NiFe LDH@NiCoP/NF catalyst exhibited outstanding OER and HER performance, requiring only 281 and 102 mV, respectively, to achieve 100 and 10 mA cm −2 , and also exhibited a cell voltage for overall water splitting of 1.56 V at 10 mA cm −2 .
研究领域:
电化学
·
材料科学
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催化
·
能源存储与转换
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xinhui Zhang,Aiping Wu,Dongxu Wang,Yanqing Jiao,Haijing Yan,Chengxu Jin,Ying Xie,Chungui Tian
The easily coupled HER and OER catalysts are highly desired for the hydrogen evolution by overall water splitting. Here, we design and synthesize Co-Mo based catalysts with adjustable electronic structure by tuning the Mo/Co ratio to give easily coupled, effective HER/OER catalysts. At lower Mo/Co ratio, the Mo component can move up the d-band center of the catalysts, rendering an enhanced capability of activating H 2 O to improve OER performance with a low overpotential of 223 mV at 10 mA cm −2 (η 10 ). Contrastingly, the Co component in the catalyst with higher Mo/Co ratio can induce the downward shift of the d-band center, optimizing the Gibbs free energy of hydrogen adsorption to enhance the HER activity (a low η 10 of 52 mV). These HER and OER catalysts with similar components can be coupled for overall water splitting. The electrolyzer can be driven by a solar panel to achieve effective H 2 production.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Guijun Li,Yibo Tang,Tiantian Fu,Yang Xiang,Zhongping Xiong,Yujun Si,Chaozhong Guo,Zhiqiang Jiang
The development of efficient and cost-effective bifunctional electrocatalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is crucial for the commercialization of rechargeable metal-air batteries. Herein, the pyrolysis of a precursor containing g-C 3 N 4 , thiourea, cobalt chloride and ferric chloride was used to fabricate S, N co-doped carbon nanotubes functionalized with Co 3 Fe 7 alloy nanoparticles (CoFe/S-N-C). The obtained CoFe/S-N-C catalyst exhibited an ORR half wave potential of 0.855 V ( vs . RHE) in 0.1 M KOH, outperforming a commercial Pt/C catalyst ( E 1/2 = 0.844 V). The catalyst also demonstrated superior OER catalytic activity (1.588 V at 10 mA cm −2 ) relative to RuO 2 in 0.1 M KOH, thus displaying outstanding bifunctional ORR and OER activity. A rechargeable Zn-air battery fabricated using CoFe/S-N-C shows good very performance (maximum power density of 120 mW cm −2 with a specific capacity of 814 mAh g −1 ) which was superior to a Zn-air battery fabricated using Pt/C and RuO 2 as ORR and OER catalysts (92 mW cm −2 and 787 mAh g −1 , respectively). Further, the fabricated battery using CoFe/S-N-C showed good stability, offering a discharge voltage ∼ 1.10 V and a recharge voltage ∼ 2.15 V at 10 mA cm −2 over 300 cycles, evidence of the durability of the CoFe/S-N-C catalyst.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Boyan Dai,Xinyu Wei,Liang Chen,Xiaolong Bao,Qin Zhong,Hongxia Qu
The investigation of highly efficient metal–organic framework (MOF) electrocatalysts represents a pivotal challenge in enhancing the overall efficiency of water electrolysis. In this study, we present a co-liganding method based on molecular regulation, in which succinic (s.a), adipic (a.a), and decanedioic (d.a) acids are employed to modify the original ligand H 2 BDC-based bimetallic NiFe-MOF to obtain dual-ligand NiFe-MOF electrocatalysts with excellent OER and HER performance (NiFe-MOF s.a, NiFe-MOF a.a, and NiFe-MOF d.a). Notably, NiFe-MOF d.a performs the best, particularly in 1 M KOH solution, with an OER overpotential of 242 mV and an HER overpotential of 116 mV at a current density of 10 mA cm −2 , and it demonstrates excellent stability under alkaline conditions, outperforming several recently reported Fe/Co/Ni-based catalysts. Bader charge and Mulliken charge calculations alongside experimental characterization data indicate that long-chain dicarboxylate ligands can influence the morphology, oxygen vacancy formation, and electronic structure of NiFe-MOFs. XPS and XRD analyses after the OER reveal that the four NiFe-MOFs undergo structural reorganization, with NiFe-MOF d.a having more unsaturated metal sites and more oxygen vacancies, promoting greater conversion of the MOF to NiOOH and FeOOH, which is beneficial for improving the OER performance. The density of states (DOS) results from DFT calculations demonstrate that the d-band center of NiFe-MOF d.a is relatively low, indicating that the adsorption energy of H* is reduced, which can promote the release of H 2 . Furthermore, the hydrogen adsorption free energy (ΔG H* ) values of the Fe and Ni active sites within NiFe-MOF d.a are closer to zero, thus accelerating the HER kinetics. This work paves new pathways for realizing dual-ligand MOFs.
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Ting Wang,Bowen Li,Ping Wang,Ming Xu,Dandan Wang,Yuqi Wang,Wenjing Zhang,Chaoqun Qu,Ming Feng
Heazlewoodite nickel sulfide (Ni 3 S 2 ) is advocated as a promising nonnoble catalyst for electrochemical water splitting because of its unique structure configuration and high conductivity. However, the low active sites and strong sulfur–hydrogen bonds (S–H ads ) formed on Ni 3 S 2 surface greatly inhibit the desorption of H ads and reduce the hydrogen and oxygen evolution reaction (HER and OER) activity. Doping is a valid strategy to stimulate the intrinsic catalytic activity of pristine Ni 3 S 2 via modifying the active site. Herein, the Ni foam supported Fe and Mo co-doped Ni 3 S 2 electrocatalysts (Fe-MoS 2 /Ni 3 S 2 @NF) have been constructed using Keplerate polyoxomolybdate {Mo 72 F 30 } as precursor through a facile hydrothermal process. Experimental results certificate that Fe and Mo co-doping can effectively tune the local electronic structure, facilitate the interfacial electron transfer, and improve the intrinsic activity. Consequently, the Fe-MoS 2 /Ni 3 S 2 @NF display more excellent HER and OER activity than MoS 2 /Ni 3 S 2 @NF and bare Ni 3 S 2 @NF by delivering the 10 and 50 mA cm −2 current densities at ultra-low overpotentials of 74/175 and 80/160 mV for HER and OER. Moreover, when coupled in an alkaline electrolyzer, Fe-MoS 2 /Ni 3 S 2 @NF approached the current of 10 mA cm −2 under a cell voltage of 1.60 V and exhibit excellent stability. The strategy to realize tunable catalytic behaviors via foreign metal doping provides a new avenue to optimize the water splitting catalysts.
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PubMed
高影响因子
IONICS
·
2024
·
IF 2.4
Zhao Qiuping,Bao Lixia,Wang haibing,Dou Di,Cong Yuanyuan,Li Chunlei
Preparation of an advanced bifunctional oxygen electrocatalyst is important for fuel cells, water splitting, etc. Herein, we report an oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) electrocatalyst with CoNi alloy nanoparticles uniformly distributed on nitrogen-doped carbon (N–C) nanospheres through a simple melamine-assisted pyrolysis strategy, in which a soft template approach is employed to prepare wrinkled N–C nanospheres. The Co 3 Ni 1 -N–C electrocatalyst exhibits higher onset potential (E 0 = 0.960 V vs. RHE (Reversible hydrogen electrode)), half-wave potential (E 1/2 = 0.81 V vs. RHE), and limiting diffusion current (j L = 5.5 mA cm −2 ) for ORR. Meanwhile, Co 3 Ni 1 -N–C electrocatalyst has a lower overpotential of 0.360 V vs. RHE at 10 mA cm −2 for OER, and a lower value for Tafel slope of 100 mV dec −1 , a potential difference between OER and ORR (ΔE = E j=10 -E 1/2 ) with a ΔE value of 0.779 V vs. RHE, which is close to the benchmark ΔE value of the combination of commercial noble metal catalysts (Pt/C-RuO 2 , 0.744 V vs. RHE). In addition, Co 3 Ni 1 -N–C also shows remarkable stability, maintaining a relative current of 81.45% after 10 h at 0.8 V. The relative current of Co 3 Ni 1 -N–C is also found to be stable, superior to commercial Pt/C by 34.5%. These excellent properties are due to its unique wrinkled structure, large surface area, and high content of CoNi-Nx and pyridine nitrogen active centers.
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高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Lixiong Xu,Shuo Geng
Electrocatalytic glycerol oxidation reaction (GOR) coupled with hydrogen evolution reaction (HER) is an ideal method to achieve efficient hydrogen production. However, realizing the stable degradation of glycerol to formate at high current densities still faces great challenges, mainly stemming from the competition between GOR and oxygen evolution reaction (OER) at high potentials. To address this issue, in this study, S–Cu–Ni/NF catalysts were successfully synthesized using Cu–Ni/NF catalysts as precursors. The introduction of Cu effectively suppressed the OER, enabling the catalysts to achieve more than 75% formate Faraday efficiency over a wide potential range from 1.3 V vs RHE to 1.6 V vs RHE. Meanwhile, S doping significantly enhanced the electron transport ability of GOR, enabling the S–Cu–Ni/NF catalyst to achieve a high current density of 100 mA cm–2 at a low potential of 1.395 V vs RHE. In addition, after 24 h of continuous operation at a high current density of 100 mA cm–2, the catalyst potential increased by only 40 mV, demonstrating excellent stability. Scanning electron microscopy with energy dispersive spectra (SEM-EDS), X-ray photoelectron spectra (XPS) and in situ Raman characterization confirmed that the precipitation of S promoted the formation of the active site NiOOH and its dynamic growth during the GOR process. The present study not only improved the selectivity of formate at high potentials by inhibiting OER but also significantly enhanced the GOR performance, demonstrated the potential of stable degradation of glycerol at high current densities, and provided a feasible strategy for the industrial application of glycerol oxidation coupled with hydrogenolysis.
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高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2020
·Vol. 167
·期 16
·160536
·
IF 3.721
Yizhao Tang,Hao Cheng,Qinggang He,Hanyu Li,Yue An,Jian Xie,Ronghai Liu
Through a facile, stepwise approach that includes electropolymerization, calcination, a hydrothermal method and low-temperature adsorption, a carbon array was coated with RuO2/MnO2 to form a highly efficient composite catalyst (RuO2/MnO2@carbon array) for Li–O2 batteries. The unique, hierarchical, three-dimensional array-type structure facilitates electrode wetting and oxygen transport as well as providing a large volume for Li2O2 loading. The growth of MnO2 nanosheets on the carbon array surface alters the surface roughness and provides attachment sites for the subsequent loading of catalyst nanoparticles. In addition, the introduction of RuO2 induces the formation of Mn3+ on the surface of MnO2, which not only improves the electrode conductivity but also the catalytic activity for ORR/OER. As a result, conformal growth of thin layers of Li2O2 on the surface of the RuO2/MnO2@carbon array and reversible decomposition of Li2O2 during cycling were achieved. In comparison with cathodes without a carbon array or catalyst, the Li–O2 cell with a RuO2/MnO2@carbon array cathode exhibits an markedly improved performance with high discharge capacity (10 000 mAh g−1 at 100 mA g−1) and long cycling life (252 cycles at 200 mA g−1 with a limited capacity of 500 mAh g−1).
研究领域:
材料科学
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电化学
·
能源存储
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高影响因子
Nanoscale
·
2022
·Vol. 14
·期 46
·17447-17459
·
IF 8.307
Wenhao Tang,Jialin He,Kewei Teng,Lei Gao,Ruiyu Qi,Yirui Deng,Ruiping Liu,Ang Li,Huadong Fu,Chang-an Wang
3d Transition-metal nitrogen–carbon nanocomposites (T–N–C, T = Fe, Co, Ni, etc.) with highly active M–Nx sites have received much attention in the field of rechargeable zinc–air battery research. However, how to rationally dope metallic elements to decorate T–N–C catalysts and enhance their electrocatalytic performances remains unclear. Herein, we demonstrated that cobalt-doped Fe-rich catalysts are effective in improving ORR performances by density functional theory (DFT) calculations. On this basis, we reported a kind of novel bifunctional electrocatalyst of hollow nitrogen-doped carbon tubes with coexisting M–N–C single atoms and alloy nanoparticles (denoted FexCoyNiz@hNCTs). Benefiting from the synergistic effect between different components, the as-prepared Fe4Co1Ni2@hNCT catalyst exhibited a small overpotential difference of 0.75 V between an OER potential at 10 mA cm−2 and an ORR half-wave potential, as well as an excellent zinc–air battery performance, when serving as the air cathode. This work provided a scalable design concept for multi-metal doping toward high-performance T–N–C electrocatalysts.
研究领域:
电化学
·
材料科学
·
能源存储
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Zuyang Luo,Qimin Peng,Zhiyang Huang,Lixia Wang,Yuting Yang,Jiaxin Dong,Tayirjan Taylor Isimjan,Xiulin Yang
Developing high-activity, long-durability, and noble metal-free oxygen evolution (OER) and hydrogen evolution (HER) cocatalysts are the bottlenecks for efficient overall water splitting (OWS). Here, novel cobalt vanadium oxides doped by nitrogen were synthesized by nitriding Co 2 V 2 O 7 @NF precursor at 300–450 °C for OER and HER reactions. N-Co 2 V 2 O 7 @NF (350 °C) and N-Co 2 VO 4 /VO 2 @NF (400 °C) show remarkable OER and HER performance with overpotentials of 310 mV and 224 mV at high current density (100 mA cm −2 ). Besides, they also revealed long-term solid stability even after 170 h and 700 h of continuous performance. Furthermore, the N-Co 2 V 2 O 7 @NF (+) ||N-Co 2 VO 4 /VO 2 @NF (–) OWS device possesses a cell voltage of 1.93 V at 500 mA cm −2 better than RuO 2 @NF (+) ||Pt/C@NF (–) (2.02 V) and can operate for 60 h with almost no degradation. This extraordinary performance can be attributed to the nanosheet structure, which can maximize the exposure of active sites and accelerate the mass transfer. Moreover, density functional theory (DFT) calculations suggest that N -doping can fine-tune the d-band center and band gap to facilitate intermediate adsorption and electron motion. The method presented here can be applied in other novel N -doped electrocatalysts for the energy field.
研究领域:
材料科学
·
电化学
·
能源材料
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DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Luyao Shi,Qinyuan Yu,Ziqi Guo,Xuedong Wei
The composite electrocatalyst of Ni(OH)₂@Fe-BDC@ Fe 3 O 4 /NF was successfully prepared. • The Ni(OH)₂@Fe-BDC heterostructure and dispersed Fe 3 O 4 nanoparticles optimize electron transfer pathways. • It is outstanding catalyst with the overpotential of 149 mV at 10 mA·cm⁻². • It has durable OER life with nearly 100 h under initial 110 mA·cm −2 . • It possesses equally excellent HER and overall water splitting performance. Metal-organic frameworks (MOFs) have gradually become highly promising electrocatalytic materials applied in the reaction of oxygen evolution (OER), thanks to their extraordinarily high specific surface area, adjustable pore structure as well as ample redox active sites. However, their practical applications are hindered by intrinsically low electrical conductivity and inadequate cycling stability. The present research introduces a brand-new Ni(OH) 2 @Fe-BDC@Fe 3 O 4 /NF nanocomposite electrocatalyst that was successfully prepared via a stepwise solvothermal method on a Ni foam (NF) support. Systematic structural characterizations confirmed that Ni(OH) 2 nanosheets in the composite exists as a mixture structure of honeycomb-like and flower-cluster-like, which uniformly anchored at the surface of Fe-BDC@Fe 3 O 4 /NF. Moreover, the coexistence of Ni(OH) 2 , Fe-BDC and Fe 3 O 4 three phases was verified in the composite. And Fe 3 O 4 nanoparticles are evenly dispersed in Fe-BDC crystal nanolayers. Electrochemical tests in 1 mol/L KOH alkaline electrolyte demonstrated that the Ni(OH) 2 @Fe-BDC@Fe 3 O 4 /NF composite exhibited superior OER catalytic activity and complete hydrolysis performance compared with the single-component Ni(OH) 2 /NF and Fe-BDC@Fe 3 O 4 /NF, delivering an overpotential as low as 149 mV under a current density of 10 mA·cm −2 , alongside a full water decomposition voltage of 1.53 V at 50 mA·cm −2 . The improved performance stemmed from the strong interfacial electronic interaction between Ni(OH) 2 and Fe-BDC@Fe 3 O 4 , which induced a negative shift in the binding energies of Ni 2p and Fe 2p, increased the interfacial charge density, reduced the charge transfer resistance (Rct = 0.8 Ω) and enlarged the electrochemical specific surface area (ECSA). In addition, the composite showed excellent long-term durability, with only 8.30% activity decay following 100 h of non-stop chronoamperometry testing under initial current density of about 110 mA·cm −2 . Structural evolution analysis after the stability test revealed that the Fe 3 O 4 phase underwent reductive decomposition and in-situ reconstruction with Ni(OH) 2 to form amorphous Ni- Fe oxyhydroxide, which served as the real active sites. This research offers a feasible approach for the structural design of iron-based MOF composite electrocatalysts, deepens the understanding of the role of interfacial synergetic mechanism between metal hydroxides and MOFs in improving OER performance, and offers experimental evidence for the advancement of high-performance non-noble metal electrocatalysts applied in water electrolysis. Download: Download high-res image (202KB) Download: Download full-size image
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