CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Xiang Li,Lu Wang,Ruiying Li,Ming Ke,Ying Zhou,Jian Liu
Developing efficient and economical electrocatalysts for hydrogen evolution reaction (HER) over a broad pH range has received considerable attention. In this work, we prepared multi-dimensional MoS 2 /S-CoP heterojunction catalysts by utilizing the carbon clothes supported ZIF-67 array as templates combining with Mo-ion exchange and high-temperature phosphorization-sulfidation strategy. The introduction of MoS 2 into S-CoP results in electron redistribution and the formation of a distinctive space charge region at the two-phase contact interface, thereby effectively tuning surface properties, enhancing electron conductivity, and improving electrocatalytic activity. According to Density Functional Theory (DFT) calculations, the introduction of MoS 2 is advantageous for the adsorption and desorption of H*, resulting in the value of ΔG H* very close to zero. Furthermore, the adsorbed water molecules are more readily activated, rendering the ΔG H2O-dis decrease, thus significantly promoting HER activity. These features contribute to robust HER electrocatalytic performance in a wide pH range and even in seawater, which is also beneficial for industrial applications. In particular, MoS 2 /S-CoP exhibits superior HER performance in alkaline seawater, requiring only 197 and 228 mV to reach the current densities of 100 and 200 mA cm -2 , respectively. This study offers novel perspectives on high-performance heterostructures for HER electrocatalysts in alkaline seawater environments.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Xiaolan Tang,Na Yang,Zixiao Li,Zhengwei Cai,Qiuying Dai,Hefeng Wang,Xun He,Yongchao Yao,Tingshuai Li,Jun Guo,Xiaobin Niu,Xuping Sun
Seawater splitting is increasingly recognized as a promising technique for hydrogen production, while the lack of good electrocatalysts and detrimental chlorine chemistry may hinder further development of this technology. Here, the interfacial engineering of manganese dioxide nanoparticles decorated on NiFe layered double hydroxide supported on nickel foam (MnO 2 @NiFe LDH/NF) is reported, which works as a robust catalyst for alkaline seawater oxidation. Density functional theory calculations and experiment findings reveal that MnO 2 @NiFe LDH/NF can selectively enrich OH − and repel Cl − in oxygen evolution reaction (OER). MnO 2 @NiFe LDH/NF attains a current density of 1000 mA cm −2 in alkaline seawater with an ultralow overpotential of only 313 mV. Furthermore, it can maintain stability at 1500 mA cm −2 over 600 h. Further phosphidation of MnO 2 @NiFe LDH/NF can create MnO x @NiFeP/NF used in efficient hydrogen evolution reaction. Moreover, an anion exchange membrane electrolyzer with MnO 2 @NiFe LDH/NF as the anode and MnO x @NiFeP/NF as the cathode was also capable of seawater splitting at 500 mA cm −2 for 100 h. This work offers light to develop effective and long-lasting electrocatalysts for seawater splitting.
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PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Yufei Feng,Shaobo Ye,Chenchen Yue,Wenhao Liu,Xuyang Lu,Qiao Liu,Qiliang Wei,Zhisheng Wu,Weiyou Yang,Qing Shi
The construction of NiFe-based composites on foam metal is an advanced strategy to design high-performance catalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Herein, we chose Fe foam (FF) as the substrate, which was first modified by anodic electrodeposition to form a porous and loose FeS x / FeO x layer. This modified layer facilitates the construction of nanoflower-structured NiFeS 2 /NiFe 2 O 4 composites with large electrochemical active surface area, higher Ni content and enhanced ratio of Ni 3 + to Ni 2+ , compared with the sample fabricated by direct etching FF. The prepared NiFeS 2 /NiFe 2 O 4 /FF electrode only requires overpotentials of 242 and 273 mV to achieve current densities of 100 and 500 mA cm⁻ 2 for OER, respectively. It also possesses faster reaction kinetics with a low Tafel slope of 31.12 mV dec −1 and superior durability without potential reduction for 200 h at a large current density of 500 mA cm⁻ 2 . Meanwhile, the performance of overall water splitting cell assembled with NiFeS 2 /NiFe 2 O 4 /FF is better than that of cell based on the noble metal Pt/C/FF- |RuO 2 /FF. This work provides a simple and cost-effective strategy for constructing efficient electrocatalysts, making it promising for large-scale industrial applications in alkaline water electrolysis.
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高影响因子
Journal of Electrochemical Science and Technology
·
2024
·Vol. 15
·期 3
·353-364
·
IF 2.2
Baikai Zhang,Xiaohui Li,Maochang Liu
Through component regulation and morphological construction, it is of considerable significance to develop high-activity and high-stability electrocatalyst for hydrogen evolution in electrolytic water. In the hydrothermal process, Mo-doped nickel-based sulfide catalysts (Mo-NiS-Fx) with a variety of morphologies (prisms, rods, flakes, and cones) were created by adding NH4F with varying masses. Among these, the flaky Mo-NiS-F1.2 exhibited exceptional performance towards electrochemical hydrogen evolution reaction, surpassing most similar catalysts with an overpotential of 79 mV at 10 mA cm-2 and a Tafel slope of 49.8 mV dec-1. Significantly, Mo-NiS-F1.2 maintained its high activity for hydrogen evolution over 60 h at a current density of 10 mA cm-2, making it suitable for widespread commercial application. According to the experimental findings, an electrocatalyst with a high surface area and a porous structure is better suited to exposing more gas transfer routes and active sites, which would encourage the hydrogen evolution reaction. This study presents a straightforward procedure for creating electrocatalysts with a range of morphologies, which can serve as a model for the creation of catalysts for use in industrial manufacturing.
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CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Haochun Chen,Yin Wang,Shuxing Zhou,Nianpeng Li,Xijun Liu,Abdukader Abdukayum,Lei Zhang,Guangzhi Hu
The development of water-separation-performing, noble-metal-free, and cost-effective electrocatalysts is of the utmost importance. This work outlines the preparation of ordered, macroporous MoS 2 –Fe 2 Mo 3 O 8 /MoO 2 electrocatalysts with heterogeneous structures using pyrolysis and sulfidation methods. The resulting macroporous and heterogeneous structures feature more active sites and facilitate ion diffusion, thereby effectively improving the overall performance. The catalyst demonstrated excellent performance in both the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) in a 1 M potassium hydroxide solution, requiring overpotentials of 213 and 60 mV, respectively, to achieve a current density of 10 mA cm −2 . Moreover, the MoS 2 –Fe 2 Mo 3 O 8 /MoO 2 -based electrolyzer only requires an output voltage of 1.49 V, exhibiting superior performance and long-term stability compared to commercial catalysts. This study introduces a novel approach for achieving a heterogeneous macroporous structure that can enhance electrocatalysis .
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Yumin Guo,Meiran Chen,Yanjie Wang,Xianglong Lu,Jingjing Wu,Xin Tang
Zinc-air batteries (ZABs) are an emerging energy technology that is environmentally friendly and has a high theoretical energy density, but their commercial application is limited by the oxygen reduction reaction (ORR). Silver-based nanocatalysts can effectively improve the ORR performance. In this paper, a nanoporous Ag–Mn (NP-AM) electrocatalyst with bicontinuous ligaments was prepared by a combination of the melt-spinning technique and dealloying method. Theoretical calculations show that Mn-doped Ag(111) indicates a shift of the d-band center toward the Fermi energy level, which improves the adsorption energy of the OOH and thus reduces the overpotential of the decision step in the ORR process. Among them, the electrocatalyst NP-AM-5 reached a half-wave potential of 0.81 V (vs reversible hydrogen electrode (RHE)) with a limiting current density of −5.63 mA cm–2. Tests showed that its ORR process almost completely undergoes 4e– transfer with higher conversion efficiency and also exhibits better long-term stability in comparison to commercial Pt/C electrocatalysts. When used as the cathode of a zinc-air battery, the maximum power density reaches 140 mW cm–2. The discharge voltage can be maintained at about 1.2 V for a long period of time by discharging at a constant current of 10 mA cm–2, and the specific capacity is calculated to be 724 mAh g–1.
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Journal of Energy Chemistry
·
2024
·
IF 14
Yugang Qi,Qing Liang,Kexin Song,Xinyan Zhou,Meiqi Liu,Wenwen Li,Fuxi Liu,Zhou Jiang,Xu Zou,Zhongjun Chen,Wei Zhang,Weitao Zheng
Atom-level modulation of the coordination environment for single-atom catalysts (SACs) is considered as an effective strategy for elevating the catalytic performance. For the MN x site, breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way, but it remains challenging for elucidating the underlying mechanism of interaction. Herein, a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks. X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell (denoted as Co-N/P-C). The prepared catalyst exhibits excellent oxygen reduction reaction (ORR) activity as well as zinc-air battery performance. The introduction of P atoms in the Co-SACs weakens the interaction between Co and N, significantly promoting the adsorption process of *OOH, resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier, responsible for the increased intrinsic activity. Our discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yuanhua Xiao,Shiwei Zhang,Ya Shen,Jinhui Shou,Yang Kong,Dangcheng Su,Xuezhao Wang,Qingxiang Yang,Dafeng Yan,Chengguo Sun,Shaoming Fang
Co 9 S 8 has been extensively studied as a promising catalyst for water electrolysis. Doping Co 9 S 8 with Fe improves its oxygen evolution reaction (OER) performance by regulating the catalyst self-reconfigurability and enhancing the absorption capacity of OER intermediates. However, the poor alkaline hydrogen evolution reaction (HER) properties of Co 9 S 8 limit its application in bifunctional water splitting. Herein, we combined Fe doping and sulfur vacancy engineering to synergistically enhance the bifunctional water-splitting performance of Co 9 S 8 . The as-synthesized Co 6 Fe 3 S 8 catalyst exhibited excellent OER and HER characteristics with low overpotentials of 250 and 84 mV, respectively. It also resulted in the low Tafel slopes of 135 mV dec −1 for the OER and 114 mV dec −1 for the HER. A two-electrode electrolytic cell with Co 6 Fe 3 S 8 used as both the cathode and anode produced a current density of 10 mA cm −2 at a low voltage of only 1.48 V, maintaining high stability for 100 h. The results of in/ex-situ experiments indicated that the OER process induced electrochemical reconfiguration, forming CoOOH/FeOOH active species on the catalyst surface to enhance its OER performance. Density functional theory (DFT) simulations revealed that Fe doping and the presence of unsaturated coordination metal sites in Co 6 Fe 3 S 8 promoted H 2 O and H* adsorption for the HER. The findings of this study can help develop a strategy for designing highly efficient bifunctional water splitting electrocatalysts.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Jihan Wu,Ying Chang,Shaohong Guo,Aiju Xu,Jingchun Jia,Meilin Jia
Ruthenium-based nanomaterials are considered to be promising electrocatalysts for HER due to their higher activity. However, the active site exposure is low, and the catalytic mass activity is low. In order to achieve the particular aims, several types of engineering, such as crystal engineering, topography engineering, heterostructures and support engineering, have been used to catalysts. Here we report RuO 2 supported on CeO 2 -NC, owing to the abundant heterostructures and the presence of oxygen vacancies, the RuO 2 /CeO 2 -NC catalyst showed outstanding HER performance (98.2 mV, 53 mV and 298 mV@100 mA cm −2 in acidic, alkaline and neutral, respectively). Moreover, RuO 2 /CeO 2 -NC also has an excellent electrocatalytic durability for 40 h. The experimental achievements show that oxygen vacancies and heterostructures could jointly enhance performance of catalyst HER.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2024
·
IF 4.1
Boyan Ai,Guoxiang Wang,Pengchao Liang,Jinxiu Bing,Majie Zhang,Qingwang Min,Xinxin Zhang
The development of highly active and acid-stable Ru-based electrocatalysts is of great significance for water electrolysis but remains a huge challenge due to serious Ru corrosion in an acid medium. Herein, we prepared oxygen vacancy (O V )-rich Nd-doped RuO 2 nanocrystals by facile synthesis via hydrothermal and subsequent annealing for efficient overall water splitting. The catalyst exhibits an overpotential of only 200 mV for OER and 44 mv for HER at the current density of 10 mA cm −2 in 0.5 M H 2 SO 4 electrolyte. Nd-doped RuO 2 only demands a cell voltage of 1.52 V to drive the overall water splitting reaction and displays excellent stability for 100 h. Density functional theory further revealed that the newly constructed Nd-doped RuO 2 sites activate the difficult to react *O intermediates, reducing the adsorption energy of the OER intermediates to effectively minimize the Gibbs free energy (*O to *OOH) of the reaction rate-determining step and regulate the center of the active site d-band. The synergistic effect of aliovalent doping and vacancy engineering contributes to the excellent electrocatalytic performance of Nd-doped RuO 2 . This performance control strategy can pave the way for the development of effective and economically viable catalysts.
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高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Qi Ling,Kui Yan,Ziwei Zhao,Zihan Zhou,Zhaoqi Sun,Lei Yang,Miao Zhang
Due to the growing demand for clean renewable hydrogen fuel , the rational design of electrode materials' composition and structure holds significant importance in achieving efficient energy storage and conversion in electrochemical energy devices. In this study, we synthesize NiCo-MOF74/NF substrate using a one-step hydrothermal method , after which we successfully deposit a layer of Ru metal nanoclusters on the substrate by electrodeposition . Ru NCs@NiCo-MOF74/NF exhibits an exceptionally large specific surface area and excellent interface effects, demonstrating outstanding performance in both overall water splitting and supercapacitor applications. In a 1 M KOH alkaline solution, the device requires only 1.47 V output voltage to deliver a current density of 10 mA cm −2 for overall water splitting. As a supercapacitor , the unique nanoflower structure of Ru NCs@NiCo-MOF74/NF enables fast and reversible Faradaic reactions, providing high specific capacitance and rate performance. It shows a high areal capacitance of 1.664 mAh cm −2 at 1 mA cm −2 , indicating excellent charge storage capacity. Assembled into an asymmetric supercapacitor (ASC) with Ru NCs@NiCo-MOF74/NF as the positive electrode , the device achieves a high energy density of 511.88 μWh cm −2 at a power density of 545.68 μW cm −2 . After 5000 cycles, the capacitance retention rate is approximately 100 %, demonstrating remarkable cycling stability. This paves the way for the synthesis of multifunctional catalysts, opening up new possibilities in the field.
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ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Yanli Niu,Xiaoqin Huang,Lei Zhao,Weihua Hu,Chang Ming Li
We herein report a facile strategy to synthesize transition metal/spinel oxide nanoparticles coupled with nitrogen-doped graphene (Co/CoFe2O4@N-graphene) as an efficient bifunctional electrocatalyst toward the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). This approach involves a spontaneous solution-polymerization of polydopamine (PDA) film on graphene oxide (GO) sheets in the presence of Fe3+ and Co2+ to form the Fe/Co-PDA-GO precursor, followed by pyrolysis at 800 °C in argon (Ar) atmosphere. During the calcination process, Co/CoFe2O4 nanoparticles are in situ formed via high-temperature solid state reaction and are further entrapped by the PDA-derived N-doped carbon layer. As-prepared Co/CoFe2O4@N-graphene exhibits highly efficient catalytic activity and excellent stability for both ORR and OER in alkaline solution. This work reports a facile synthetic approach to develop highly active electrocatalysts while offering great flexibility to tailor their components and morphologies and thus provides a useful route to the design and synthesis of a broad variety of electrocatalysts.
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