JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Yuxuan Shao,Junjie Ni,Jie Yin,Xinqing Liu,Yulai Song,Yue Xu,Shuai Guo,Laima Luo
The construction of heterojunctions between non-noble-metal based compounds affords a scheme for accelerating the reaction kinetics of oxygen evolution reaction (OER) without using precious mental materials, which is extremely important but remains challenging. Herein, the heterogeneous structure between Fe 60 Co 10 Ni 10 Cr 10 Mn 10 medium-entropy alloy (MEA) and FeS 2 is developed by a mechanical alloying approach. The resulting MEA-30 wt%FeS 2 delivers a high OER activity with a low overpotential of 261.6 mV at 10 mA/cm 2 , along with Tafel slope of 52.7 mV/dec in 1.0 mol/L KOH solution, superior to the commercial RuO 2 . The combination of detailed characterization techniques and density functional theory (DFT) calculation reveals that the heterojunctions between Fe-based MEA and FeS 2 generates the synergistic effect on the activation and formation steps of OOH*, thus promoting the OER reaction kinetics. Furthermore, the abundant active sites provided by the reconstructions of MEA-30 wt%FeS 2 during OER process also contributes to the catalytic performance. This work greatly expands the application scope of medium-entropy materials and provides a new method for the fabrication of novel heterogeneous electrocatalyst of Fe-based MEA and FeS 2 .
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
·
IF 8.1
Zeting Deng,Xiangbowen Du,Kaicheng Qian,Leilei Du,Zheng Fang,Jiayang Zhu,Jia Hong,Feng Wang,Tongtong Li,Tong Wei,Renhong Li
The conventional anodic oxygen evolution reaction (OER) can be ideally replaced by the urea oxidation reaction (UOR) to achieve efficient hydrogen generation due to the superior thermodynamics. However, the UOR involves a slow 6-electron transfer dynamic, necessitating the utilization of high-performance catalysts to enhance catalytic efficiency. In this work, a bifunctional transition metal-based catalysts, namely, MoO 2 –NiO/NF heterostructure, is effectively synthesized using two-step hydrothermal methods and calcination. Benefiting from the heterogeneous interface, the nanoflower-like structure as well as the electron density redistribution, the MoO 2 –NiO/NF catalyst demonstrates remarkable durability and performance, with an overpotential of 139 mV to achieve 10 mA cm −2 for UOR. In addition, the bifunctional catalyst is used in a two-electrode electrolyzer, where a current density of 10 mA cm −2 is attained at a potential of 1.317 V, which is 261 mV smaller than that of the conventional water splitting system. Based on the density functional theory (DFT) calculations, the MoO 2 –NiO/NF heterostructure exhibits a higher density cloud in the vicinity of the Fermi level, revealing that it has faster electron transfer and higher electrical conductivity. Besides, the Mo sites and Ni sites are favorable for adsorption of CO(NH 2 ) 2 and H 2 O, respectively, which might optimize the reaction intermediates adsorption/desorption for UOR/HER, ultimately leading to the high electrocatalytic performance of MoO 2 –NiO/NF. This research opens a new window for the development of advanced heterojunction electrocatalysts assisted by urea electrocatalysis for cost-effective hydrogen production.
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FUEL
·
2024
·
IF 6.7
Wenfeng Peng,Zhengxing Lv,Wenju Zhou,Bingmin Yan,Shijing Zhao,Lailei Wu,Junshuang Zhou,Huiyang Gou
Creating highly efficient bifunctional transition metal phosphide catalysts for electrochemical water splitting through cost-effective and universal methods remains an elusive challenge. Here we introduce a universal high temperature and high pressure (HTHP) technique that readily produce phase-pure TMPs, including FeNiP, CoNiP, and Fe 2/3 Co 2/3 Ni 2/3 P (CFNP), which can serve as an ideal model for investigating the relationship between electrocatalytic activity, structure, and chemical composition. The crystal structure of obtained CFNP has been carefully determined for the first time by using single-crystal X-ray diffraction (XRD) and XAS simulations. In the structure of CFNP, iron atoms form an MP4 tetrahedron with Co atoms and a 5-coordination pyramid with Ni atoms. This arrangement synergistically induces an electron-deficient state in the metals and an electron-rich state in phosphorus, enhancing CFNP/NF’s bifunctional catalytic effectiveness, achieving low overpotentials of 92 mV and 239 mV at 10 mA/cm 2 in 1 M KOH environment for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively. Moreover, an integrated electrolyzer using CFNP/NF as both electrode components can achieve a current density of 10 mA cm −2 at 1.536 V, showcasing a catalytic activity for overall water splitting comparable to those of phosphide-based electrocatalysts. The HTPH technique opens new possibility for exploring pure-phase multimetallics and high-entropy phosphides as potential multifunctional materials for potential applications.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Fengxin Cao,Qiaoling Li,Boya Shan,Zhiwei Qi,Chenyu Zhang,Chengcheng Yu
To create an economical, stable, along highly efficient catalyst for the hydrogen evolution reaction, this paper reports on a Cr-doped self-supported Co-P-Cr/NF high-performance HER catalyst synthesized in one step. It exhibits overpotentials of 41.44 mV at −10 mA cm −2 . Moreover, the impedance is only 0.56 Ω, and the double-layer capacitance value is 40.02 mF cm −2 . After a 12-hour stability test, the catalyst shows only minimal overpotential increase. Using techniques including XRD, XPS, SEM, and TEM, the structure of the electrocatalyst was thoroughly investigated. The introduction of Cr and the excellent electronegativity of P enhance the redox capability and show superior intrinsic electrocatalytic ability in Co-P-Cr/NF catalysts. Therefore, the Co-P-Cr/NF catalyst that has been developed shows promise in replacing costly Pt-based electrocatalysts in the HER.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2024
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IF 4.1
Mohib Ullah Khan,Afaq Ullah Khan,Sameerah I. Al-Saeedi,Kamran Tahir,Abdulaziz A. Alanazi,Zainab M. Almarhoon,Talal M. Althagafi,Magdi E.A. Zaki,Hassan M.A. Hassan,Mingzai Wu
A binary composite of metal sulfides (MS) is directly synthesized on nickel foam through hydrothermal process, resulting in snow like nanosphere suitable for hybrid supercapacitors (HSCs). Herein, a ZnS/CdS binary composite has been grown directly on nickel foam using a simple hydrothermal method. The structural features, morphological characteristics and electrochemical performance of the composite are systematically investigated. Especially, the highest capacitance of 739–325 F/g at 1–10 A/g was attained with good rate performance. Moreover, a binder-less ZnS/CdS/NF composite achieved a high power of 5030 W/kg at 42 Wh/kg energy density by realizing an expanded voltage to 1.8 V with decent durability. Interestingly, a 92.84 % retention was noticed after 6500 cycles, which indicates high performance stability of the ZnS/CdS/NF||AC HSC. These outcomes reveal the promising prospect of all-metal sulfide utilization for next-generation energy storage devices.
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Water
·
2024
·Vol. 16
·期 22
·3235
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IF 3
Qiao Xu,Fenfen Yan,Yujie Fan,Miao Gong
This work evaluated the alterations in the levels and types of polycyclic aromatic hydrocarbons (PAHs) within both liquid and solid products throughout the process of the catalytic supercritical water gasification of dewatered sewage sludge to examine the catalytic effect of various catalysts and the inhibit reaction pathways. The addition of Ni, NaOH, Na2CO3, H2O2, and KMnO4reduced the concentrations of PAHs, with Ni and H2O2showing the best performance. The concentrations of PAHs, especially higher-molecular-weight compounds in the residues, decreased sharply as the H2O2amount increased. At a 10 wt% H2O2addition, the levels of PAHs in the liquid and solid products were reduced by 91% and 88%, respectively. High-ring PAHs were not detected in the residues as the H2O2amount increased to an 8 wt%. H2O2addition evidently inhibits PAH formation by promoting the ring-opening reactions of initial aromatic compounds in raw sludge and inhibiting the polymerization of open-chain intermediate products. The addition of NaOH + H2O2or Ni + H2O2as combined catalysts significantly lowered PAH concentrations while increasing the H2yield. The addition of 5 wt% Ni + H2O2reduced PAH concentrations in the liquid and solid residues by 70% and 44%, respectively, while the H2yield escalated from 0.13 mol/kg OM to 3.88 mol/kg OM. Possible mechanisms associated with the reaction pathways of these combined catalysts are proposed.
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MOLECULES
·
2025
·Vol. 30
·期 1
·177
·
IF 4.6
Zhi Lu,Yifan Guo,Shilin Li,Jiaqi Ding,Yingzi Ren,Kun Tang,Jiefeng Wang,Chengxin Li,Zishuo Shi,Ziqi Sun,Hongbo Meng,Guangxin Wang
Water electrolysis is a promising path to the industrialization development of hydrogen energy. The exploitation of high-efficiency and inexpensive catalysts become important to the mass use of water decomposition. Ni-based nanomaterials have exhibited great potential for the catalysis of water splitting, which have attracted the attention of researchers around the world. Here, we prepared a novel Mo-doped NiFe-based layered double hydroxide (LDH) with a nanoarray microstructure on Ni foam. The doping amount of Mo can significantly change the microstructure of the electrocatalysis, which will further affect the oxygen evolution reaction (OER) performance of water splitting. This novel nanomaterial required only an overpotential of 227 mV for 10 mA cm−2and a Tafel slope of 54.8 mV/dec in 1 M KOH. Meanwhile, there was no Mo, and the NiFe-LDH needed 233 mV to attain to 10 mA cm−2. Compared to the NiFe-LDH without Mo, the NiFeMo-LDH nanosheet arrays exhibited enhanced activities with 17.1 mV/dec less Tafel in OER. The good performance of the electrocatalyst is ascribed to the special nanosheet arrays and the heterostructure of the Ni-Fe-Mo system. These features help to increase the active surface, enhancing the efficient charge transfer and the reactive activity in OER.
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Materials Today Physics
·
2024
·
IF 10
Yuping Duan,Meiqi Li,Yuan Guo,Ning Zhu,Huifang Pang,Chenxu Dou
High-entropy alloys, as a novel type of absorber, exhibit exceptional electromagnetic modulation capabilities and significant potential for electromagnetic wave absorption. In this work, the FeCoNiCrMn high-entropy alloy absorbent prepared through a mechanical alloying process demonstrates a dual-phase solid solution structure comprising face-centered cubic (FCC) and body-centered cubic (BCC) phases. By varying the manganese (Mn) content in the system, it is possible to enhance the degree of crystallinity, maintain the integrity of the crystal structure, and effectively control the relative proportion of the BCC phase within the overall phase composition. This adjustment improves the brittleness of the sheet-like particles, reduces particle size, and significantly lowers the permittivity. When the molar ratio of Mn is 0.6, the sample exhibits improved impedance matching due to the optimal permittivity and permeability. Notably, the impedance matching and attenuation constant can also be balanced. At 6.42 GHz, the FeCoNiCr 0.4 Mn 0.6 alloy powder achieves the maximum reflection loss of −48.49 dB at a matching layer thickness of 3 mm. When the matching thickness is reduced to 2 mm, it can effectively cover a frequency range of 8.7–14.1 GHz (effective absorption bandwidth of 5.4 GHz), along with a wide absorption bandwidth and high absorption efficiency.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jiaxing Song,Jiabao lv,Yuhan Pan,Jingyu Wang,Jun Wang,Ang Cao,Angjian Wu,Paul T. Williams,Qunxing Huang
Conventional catalytic pyrolysis of waste plastics for H 2 production faces challenges due to excessively high reaction temperatures. This study introduced a NiCeOx/β catalyst for low-temperature H 2 production from polyethylene (PE), aiming to enhance H 2 yield through nonthermal plasma (NTP) and catalytic active sites. Experimental results confirmed the efficacy of NTP in promoting collision between high-potential-energies active species and plasma-catalyst interactions, identifying acidic sites as primary catalytic active sites. Both experiments and density functional theory (DFT) calculations confirmed NiO and CeO 2 particles as metallic active sites, exhibiting thermodynamic and kinetic benefits for primary products from PE pyrolysis. Under optimal conditions, the highest H 2 yield and selectivity respectively reached 32.71 mmol/g and 82.10 % at a PE/(NiCeOx/β) ratio of 1:4, reaction temperature of 400 °C, and NTP discharge power of 210 W. The NiCeOx/β catalyst facilitated low-temperature pyrolysis of waste plastics, enhancing H 2 selectivity and yield.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Mingchong Sui,Fangqing Wang,Caichi Liu,Qiuyan Hao,Ying Li,Hui Liu,Limin Liang
Cobalt–iron layered double hydroxide (CoFe LDH) is considered an advanced electrocatalyst toward the alkaline oxygen evolution reaction (OER), yet its poor stability is still a huge challenge. Here, based on an innovative spontaneous redox reaction (SRR) method, we synthesize a gold-nanoparticle-decorated CoFe LDH heterostructure on nickel foam (Au/CoFe LDH/NF) at room temperature. The heterostructure catalyst not only exhibits a low overpotential of 233 mV at 10 mA cm–2 but also displays 400 h stability without any degradation at ∼200 mA cm–2. The experimental and density functional theory (DFT) calculations validate that Au/CoFe LDH/NF with strong electronic coupling at the interface optimizes the electronic structure, reducing the OER energy barrier. In situ Raman spectra demonstrate that the transfer of electrons from Au nanoparticles to CoFe LDH alleviates the structural distortion of the catalyst during the OER, which is responsible for the strengthened stability.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·
IF 3.9
Junyi Chen,Jing Wang,Dongsheng Lou,Yingying Xiang,Tongming Sun,Yanfeng Tang,Minmin Wang
FeOOH with excellent catalytic properties for oxygen evolution and also considered to be a true active site has attracted great interest in recent years. However, the intrinsic low conductivity limits its catalytic performance. Herein, a one-dimensional core-shell NiMoO4/FeOOH heterojunction with high OER activity and stability was developed. At current densities of 10 and 100 mA cm-2, low overpotentials of 194 and 266 mV are need to drive oxygen evolution, meanwhile, the electrode exhibits high catalytic kinetics with small Tafel slopes of 53.4 mV dec-1 and excellent stability over 100 hours. Further analysis showed that the ultrathin FeOOH layer (~5 nm) uniformly covered the surface of NiMoO4 nanorods, acting as an active species and facilitating the surface change transfer to the interior. The internal NiMoO4 cores, on the other hand, provides reliable electron transmission as a highly conductive medium, and can effectively overcome the low conductivity of FeOOH. DFT calculations further manifest the strong electronic interactions between NiMoO4 and FeOOH species. The NiMoO4 core serves as mass transport of active materials is beneficial to tune the adsorption energy of OH- on the surface of electrocatalysts.
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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Uddin Sk Raihan,Jingqi Zhang,Jingbo Chao,Qing Hu,Frederic Coulon,Xiao Jin Yang
Chlorinated phenols are highly toxic to human and ecosystem and their biological degradation is difficult. In this work, a novel MgAlNi alloy catalyst was developed for rapid chemical degradation of p-chlorophenol (4-CP) in water under mild conditions via in situ hydrodechlorination ( i HDC) without external hydrogen gas supply. A complete conversion of 0.195 mM 4-CP to phenol was achieved within 15 min with a reaction rate constant of 7.65 h −1 , 19.4 times higher than that of the traditional Raney Nickel (AlNi alloy) catalyst. The excellent performance of MgAlNi alloy catalyst is attributed to enhanced H 2 generation by Mg etching, surface self-reconstruction by growth of in situ layered double hydroxide ( i LDH) nanosheets of 0.08–1 nm, exposed active sites of AlNi intermetallic compounds Al 3 Ni 2 and Al 3 Ni. The findings of this study provide new insights into broader applications of nanoconfinement catalysis to environmental remediation and open a new domain of in situ nanoconfinement catalysis ( i NCC).
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