Surfaces and Interfaces
·
2025
·
IF 6.3
Tianping Wang,Yining Liang,Lin Xu,Xikui Liu,De Ning,Zhengjian Chen
Precisely modulating active sites to achieve high-performance catalysts remains a significant challenge but is critical to metal-air batteries and fuel cells. In this study, core-shell structured Co-TPG-IPOF/KB containing single cobalt (Co) atoms are anchored onto a 1,3,5-triformylphloroglucinol (TPG)- based ionic porous organic framework (IPOF) coated on Ketjenblack carbon (KB) was prepared through in-situ Schiff-base condensation. Systematic experimental characterizations reveal that KB cores provide abundant mesopores and greatly increase the accessible surface area from 48 to 614 m 2 g -1 , and the Co 2+ active sites are asymmetrically coordinated and uniformly dispersed upon the surface rather than inside the bulk. These remarkable structures enable Co-TPG-IPOF/KB to exhibit excellent oxygen reduction reaction (ORR) performance with a half-wave potential of 0.842 V, superior durability and methanol tolerance, and a favorable four-electron (4e - ) pathway, and therefore Zn-air batteries catalyzed by Co-TPG-IPOF/KB achieved considerably improved maximum power density (189 mW cm -2 ), specific capacity (727 mAh g zn -1 ), and cycling energy efficiency, superior to the benchmark Pt/C catalyst.
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WATER RESEARCH
·
2025
·
IF 12.4
Huanran Liu,Qinyan Yang,Chen Wang,Yang Wu,Li Liu,Guoqing Shen,Qincheng Chen
Microbial fuel cells (MFCs) offer great potential for simultaneous wastewater treatment and energy generation, yet the development of cost-effective and efficient carbon-based cathode alternatives to Pt/C for oxygen reduction reactions remains challenging. This study presents a novel single-atom Fe-decorated N-doped porous carbon (Fe-SA/NBC) synthesized from biogas residue for wastewater treatment. The Fe-SA/NBC demonstrated superior catalytic performance, achieving a kinetic current density of 18.89 mA·cm - ² compared to 10.38 mA·cm - ² for Pt/C, and an enhanced electrochemical surface area with a C dl of 1.81 mF·cm - ² versus 1.76 mF·cm - ² for Pt/C. When integrated into an MFC air-cathode under actual sewage, Fe-SA/NBC outperformed Pt/C, achieving a 22.6 % higher power density (882.92 mW·m - ² vs. 719.81 mW·m - ²), a higher output voltage (0.53 V vs. 0.47 V), and a longer operational duration (3.6 days vs. 3.2 days). Additionally, Fe-SA/NBC exhibited superior removal efficiencies for chemical oxygen demand and ammonia nitrogen during sewage treatment. In practical applications, MFCs equipped with Fe-SA/NBC successfully powered diodes and timers in series-connected configurations. This study introduces an innovative method for producing cost-effective and efficient cathode catalysts from waste biomass, offering significant potential for wastewater treatment and power generation systems.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Zhou Yang,Nan Jiang,Shaoyi Bei,Keyan Bao,Meng Xiang,Chengbin Yu,Shuang Dong,Hengfei Qin
Searching for an excellent bifunctional electrocatalyst used in zinc-air batteries (ZABs) is a long-term and challenging task. Single-atom catalysts have been becoming potential bifunctional electrocatalysts because of their maximum metal atom utilization and low content of metal itself. Herein, noble metal palladium (Pd) is uniformly anchored in the supported WO 2.72 to form single-atom Pd/WO 2.72 owing to the special 4d orbit of Pd and nonstoichiometric 2D planar structure of WO 2.72 . Single-atom 5 % Pd/WO 2.72 is prepared in this work, showing excellent bifunctional electrocatalytic behaviors with high E 1/2 of 0.86 V for ORR and low E j= 10 of 1.59 V for OER in alkaline medium, and the ∆E is 0.73 V, which outperforms the Pt/C and RuO 2 . Furthermore, the 5 % Pd/WO 2.72 -ZAB has a high open-circuit voltage (OCV) value of 1.491 V, a large power density of 168 mW cm −2 , and a large specific capacity of 633 mAh g −1 . Besides, the 5 % Pd/WO 2.72 -ZAB also has good cycling stability.
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Catalysis Science & Technology
·
2024
·Vol. 14
·期 13
·3719-3727
·
IF 4.4
Wensheng Zhang,Xu Chen,Jinyu Zhao,Lin Niu,Guipeng Wang,Xiaomin Wang
The potential of hydrogen production via water splitting technology makes it urgent to develop low-cost and highly active bifunctional catalysts for hydrogen and oxygen evolution reactions (HER/OER). In this study, a low platinum (Pt) bimetallic phosphide heterostructure (Pt-NiFe-P/NF), derived from three-dimensional NiFe metal–organic framework (NiFe-MOF) nanorods on nickel foam (NF), was developed using a two-step hydrothermal and phosphorization process. The nickel-iron phosphide nanorod array heterostructure boasts a large surface area with numerous active sites, which enhances charge and substance transfer. The integration of metallic Pt with NiFe-P heterostructures subtly adjusts the electronic redistribution between them, thereby improving the kinetics of water splitting. Consequently, the Pt-NiFe-P/NF catalyst demonstrated exceptional HER and OER performance in a 1 M KOH solution, with overpotentials of 97 and 266 mV at 100 mA cm−2, respectively. Remarkably, an electrolyzer utilizing this catalyst requires just a 1.65 V potential to achieve a current density of 100 mA cm−2, exceeding the capabilities of conventional Pt/C||RuO2 systems, which require 2.10 V and outperforming many advanced electrochemical water splitting catalysts currently in use.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Tong Li,Lingting Ye,Kui Xie
Electrocatalytic full water splitting is still a challenge. Porous single-crystalline (PSC) has a long-range ordered crystal structure and large specific surface area , which has great potential to be applied in the fields of catalysis and energy storage. Nitride single-crystalline possesses unsaturated coordination of metal-nitrogen active sites on the crystal surface, which has shown excellent performance in the electrocatalytic field. PSC tungsten nitride mesoporous nanosheets are grown from single-crystalline (SC) WO 3 nanosheets and are applied as bifunctional electrocatalysts in Hydrogen Evolution Reaction (HER) and Oxygen Evolution Reaction (OER). The overpotential of mesoporous W 2 N and WN single-crystalline nanosheets in HER is as low as 67.44 mV and 84.26 mV at a current density of 10 mA cm −2 , respectively. A low overpotential has been found in PSC W 2 N and WN as the OER electrocatalyst . The PSC tungsten nitride mesoporous nanosheets provide a simple and effective solution for efficient water splitting electrocatalysts .
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CATALYSIS LETTERS
·
2024
·
IF 2.3
Yan Xiaoxu,Zhao Xianfeng,Shao Xinxin,Li Kangpeng,Sun Minghong,Ji Xinpeng,Lu Huidan,Liu Yongping
Platinum-group metal ruthenium (Ru) is considered an ideal substitute for platinum (Pt) in the hydrogen evolution reaction (HER) due to its excellent electrocatalytic performance and cost that is 20 times lower than Pt. Herein, we prepared Ru-doped WO 3 nanosheets array on carbon cloth (CC) using the hydrothermal method, followed by successful high-temperature nitridation to obtain Ru-WN/CC nanoarray electrocatalysts. As prepared Ru-doped WN nanosheets exhibit a highly porous structure, providing abundant active sites for HER. Electrochemical performance tests demonstrate that compared to pristine WN/CC, 7% Ru-WN/CC exhibits a reduced overpotential of 94 mV at a current density of 10 mA cm -2 , with a Tafel slope of only 51.4 mV dec -1 and an Rct of 6.08 Ω. Moreover, it maintains high catalytic activity for at least 24 hours under acidic conditions. The superior electrocatalytic activity of Ru-WN/CC is attributed to the significant acceleration of the kinetic rate of WN electrocatalysts by Ru doping, the reduction of electronic transfer resistance in WN, and the enlargement of the electrochemically active surface area of WN. This study provides an important reference for the development of novel low noble metal-doped electrocatalytic materials and has guiding significance for the application of metal nitrides in water splitting for hydrogen production. Graphical Abstract
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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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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Shan Huang,Ling-Xin Kong,Meng-Meng Wang,Hui-Hao Li,Xin-Qi Liu,Meiling Xue,Yi Fang,Ji-Sen Li,Qi Xiao
The electrolysis of seawater for hydrogen production holds promise as a sustainable technology for energy generation. Developing water-splitting catalysts with low overpotential and stable operation in seawater is essential. In this study, we employed a hydrothermal method to synthesize NiMoWO X microrods (NiMoWO X @NF). Subsequently, an annealing process yielded a composite N -doped carbon-coated Ni 3 N/MoO 2 /WO 2 nanorods (NC@Ni 3 N/MoO 2 /WO 2 @NF), preserving the ultrahigh-specific surface area of the original structure. A two-electrode electrolytic cell was assembled using NC@Ni 3 N/MoO 2 /WO 2 @NF as the cathode and NiMoWO X @NF as the anode, demonstrating exceptional performance in seawater splitting. The cell operated at a voltage of 1.51 V with a current density of 100 mA·cm −2 in an alkaline seawater solution. Furthermore, the NC@Ni 3 N/MoO 2 /WO 2 @NF || NiMoWO X @NF electrolytic cell exhibited remarkable stability, running continuously for over 120 h at a current of 1100 mA·cm −2 without any observable delay. These experimental results are corroborated by density functional theory calculations. The NC@Ni 3 N/MoO 2 /WO 2 @NF || NiMoWO X @NF electrolyzer emerges as a promising option for industrial-scale hydrogen production through seawater electrolysis.
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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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GREEN CHEMISTRY
·
2024
·
IF 9.3
Shumin Huang,Xiaolin Luo,Ji Li,Sibao Liu,Li Shuai
High-density fuel additives are important for heavy transportation. Production of high-density fuel additives from renewable resources has been receiving increasing attention in recent years. Despite the progress in the depolymerization of lignin, cellulose, and hemicelluloses, there are limited studies on integrating lignin and carbohydrates to make value-added products. Here we design a route to synthesize high-density fuel additives with lignin-derived monophenolics and carbohydrate-derived furanics. We performed Brønsted base-catalyzed C–C coupling of phenolics and furanics followed by hydrodeoxygenation catalyzed by a synthesized Ir–ReOx/SiO2 catalyst. Under optimized reaction conditions, the coupling product of phenolics and furanics, bicyclic furyl phenyl precursors, reached a yield of over 90%, and was further hydrodeoxygenated to bicyclohexyl alkanes with a yield of over 98%. The current two-step strategy demonstrates high-selectivity of preparing high-density hydrocarbon fuels from lignocelluloses and provides a possible way to utilize all components of lignocellulosic biomass in an integrated upgrading pathway.
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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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