APPLIED SURFACE SCIENCE
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2024
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IF 6.3
Yun-Yang Li,Hao-Jie Yan,Ruo-Zhan Yin,Qing-Qing Sun,Lian-Kui Wu,Fa-He Cao
In this work, SiOC coatings incorporated with Ni nanoparticles were fabricated on γ-TiAl alloy by dip-coating. The microstructure and high temperature oxidation behavior of the SiOC-Ni coatings with different Ni contents were investigated. Results showed that the incorporation of Ni nanoparticles improved the oxidation resistance of the SiOC coating at 850 ℃. During thermal exposure to air, the incorporated Ni particles would react with both oxygen and the SiOC coating, forming NiO and Ni 2 Si, respectively, therefore changing the structure of the SiOC coating. The generation of NiO and Ni 2 Si is beneficial in reducing the oxygen partial pressure at the coating/substrate interface, thereby facilitating the formation of a protective aluminum oxide layer.
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Journal of Materials Chemistry C
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2024
·Vol. 12
·期 39
·16015-16024
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IF 5.7
Jiawen Hu,Linwen Jiang,Hang Liu,Jiawei Jin,Lei Jia,Anhua Wu,Xiaofeng Zhang
Further enhancing the effective absorption bandwidth (EAB) and the harsh-environment stability of high-entropy alloy (HEA) electromagnetic-wave absorbing (EMA) materials is of great practical significance and broad application prospects. A new type of sulfur (S)-dissolved HEA EMA material was developed in this work. The flaky FeCoNiCuSx (x = 0, 0.05, 0.10, 0.20) HEAs were successfully prepared by a mechanochemical process. The phase structure, magnetic properties, corrosion resistance, oxidation resistance and EMA performances of the FeCoNiCuSx HEAs were investigated in detail and it was found that the introduction of S significantly optimized the impedance matching and achieved excellent EMA performances. The results showed that S10 (FeCoNiCuS0.10) had a minimum reflection loss (RL) of −65.20 dB and a wide EAB of 6.89 GHz. And the S20 (FeCoNiCuS0.20) achieved an ultra-wide EAB of 7.00 GHz and an RL of −55.40 dB in the C-band. In addition, the FeCoNiCuSx HEAs also exhibited excellent corrosion resistance. This work not only demonstrated the potential application of S-dissolved HEAs in the EMA field in harsh environments, but also provided new ideas for optimizing the electromagnetic impedance matching of HEAs.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Shan Xu,Dongxu Jiao,Xiaowen Ruan,Zhaoyong Jin,Yu Qiu,Jinchang Fan,Lei Zhang,Weitao Zheng,Xiaoqiang Cui
Efficient production of green hydrogen energy is crucial in addressing the energy crisis and environmental concerns. The oxygen evolution reaction (OER) poses a challenge in conventional overall water electrolysis due to its slow thermodynamically process. Urea oxidation reaction (UOR) offers an alternative anodic oxidation method that is highly efficient and cost-effective, with favorable thermodynamics and sustainability. Recently, there has been limited research on bifunctional catalysts that exhibit excellent activity for both OER and UOR reactions. In this study, we developed a selenium and iron co-doped nickel sulfide (SeFe-Ni 3 S 2 ) catalyst that demonstrated excellent Tafel slopes of 53.9 mV dec −1 and 16.4 mV dec −1 for OER and UOR, respectively. Density Functional Theory (DFT) calculations revealed that the introduction of metal (iron) and nonmetallic elements (selenium) was found to coordinate the d-band center, resulting in improved adsorption/desorption energies of the catalysts and reduced the overpotentials and limiting potentials for OER and UOR, respectively. This activity enhancement can be attributed to the altered electronic coordination structure after the introduction of selenium (Se) and iron (Fe), leading to an increase in the intrinsic activity of the catalyst. This work offers a new strategy for bifunctional catalysts for OER and UOR, presenting new possibilities for the future development of hydrogen production and novel energy conversion technologies. It contributes towards the urgent search for technologies that efficiently produce green hydrogen energy, providing potential solutions to mitigate the energy crisis and protect the environment.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Yun Tian,Jie Qu,Kejia Wu,Mengqiao Gao,Jinxing Long,Qiang Zeng,Wei Qi,Xuehui Li
Conversion of lignin to value-added chemicals with endogenous hydrogen is of great significance but highly challengeable. In this work, an external hydrogen-free strategy has been proposed for aqueous transfer hydrogenolysis of lignin launched by the chemo-splitting of water using a series of Ni-Co bimetallic catalysts. With Ni 0.2 Co 0.1 -MgAl-LDO, 82.7 % of lignin conversion was achieved, affording a 20.8 % yield of monophenols, and 62.0 % of which was identified as 4-ethylphenol (yield of 12.9 %). Further investigations demonstrated that the lignin hydrogenolysis was triggered by the water splitting, and enhanced by the tandem demethoxylation and subsequent aqueous reforming reaction. Intensive characterizations using TEM, XPS and XAFS, etc, illustrated that the formation of highly dispersed Ni-Co alloy nanoparticles exhibited a strong metal-support interaction with MgAl-LDO. The electronic transfer effect between Ni and Co components and the strong basic sites are responsible for its excellent catalytic performance of Ni 0.2 Co 0.1 -MgAl-LDO on the lignin hydrogenolysis. Therefore, this work provides novel insight into the catalytic transfer hydrogenolysis of lignin.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Riyang Shu,Yu Chen,Yuankai Lin,Yongyuan Deng,Yan Liu,Kaixin Li,Tao Yin,Zhongqing Ma,Jinxing Long
Catalytic hydrodeoxygenation (HDO) is an efficient and promising approach to upgrade lignin-derived phenolic compounds for the production of high-quality liquid fuels. In this work, a readily obtained Ni-Ni 3 P/ZrP catalyst featuring synergistic catalytic sites of Ni-Ni 3 P and Lewis-Brønsted acid was provided for promoting the HDO performance of lignin-derived phenolic compounds. By regulating the ratio of Zr to P (Zr/P), the catalytic activity of Ni/ZrP was significantly modified. With the optimized catalyst of Ni-Ni 3 P/ZrP-0.75, guaiacol is completely converted into cyclohexane at a low temperature of 240 °C. Further investigation shows that the synergistic effect of Ni and Ni 3 P, deriving from that Ni acts as metal site to activate hydrogen and Ni 3 P serves as Lewis acid site to adsorb guaiacol substrate, promotes the hydrogenation procedure significantly. Moreover, ZrP support as Lewis acid also demonstrates a synergistic interaction with Brønsted acid site that derives from the P-OH group. The coordination of Lewis-Brønsted acid site significantly improves the deoxygenation procedure. The strong interaction between Ni species and ZrP support accelerates the sequential occurrence of hydrogenation and deoxygenation procedures, thus improving the HDO efficiency. The Ni-Ni 3 P/ZrP-0.75 can be reused at least six runs without significant activity loss. Moreover, this Ni-Ni 3 P/ZrP-0.75 is efficient on the upgrading of realistic lignin-oil, with the hydrocarbon content increase from 13.4 % to 93.8 %. Therefore, this work provides a valuable reference for the rational design of bifunctional catalysts in the HDO reactions.
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ADVANCED MATERIALS
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2025
·
IF 26.8
Dashuai Li,Qi Wu,Changhua Wang,Zhehao Sun,Yingying Li,Zongyou Yin,Yichun Liu,Xintong Zhang
Transition metal high-entropy alloys (HEAs) demonstrate exceptional catalytic performance due to their structural complexity, featuring rich local atomic configurations, tunable electronic structures, and abundant active sites. However, this structural versatility poses both thermodynamic and kinetic challenges to conventional wet-chemical synthesis routes. Herein, we develop a novel solution plasma strategy that enables the direct synthesis of HEA catalysts in aqueous media. Through the FeCoNiCrMn electrode discharge in pure water, uniform HEAs nanoparticles (≈200 nm) are successfully anchored onto a variety of oxide substrates. The HEAs/TiO 2 catalyst achieves a CO generation rate of 298.1 mmol/g HEAs /h, representing ca. an order-of-magnitude higher activity than single-metal catalysts under both thermocatalytic and photothermal conditions. Advanced structural characterization reveals a dual-phase core-shell architecture consisting of a metallic alloy core and surface oxides preferentially enriched at CrMn sites. This spatially resolved structure enables cooperative catalysis, where CrMn-rich oxide domains promote H 2 dissociation, CoNi metallic regions facilitate CO 2 reduction, and Fe sites present in mixed valence states serve as electron and oxygen transfer bridges. We further identify a self-limiting oxidation mechanism intrinsic to plasma synthesis, which ensures charge redistribution at the metal-oxide interfaces and synergistically enhances photothermal catalysis. This work establishes an energy-efficient synthetic route for HEAs and elucidates structure-function relationships critical for advancing multimetallic catalytic systems.
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
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2024
·
IF 2.6
Li Gang,Ren Haifang,Geng Chunping,Wu Xiang
Electrical energy storage devices (EES) play an important role in the development of portable electronic devices, power grids, and electric vehicles. Supercapacitors (SCs) become the focus of the EES field due to their high power density and high energy density. ZnCo 2 O 4 ternary metal oxides show considerable potential as electrodes for SCs. In this work, Ni(OH) 2 and PPy materials are combined on the surface of ZnCo 2 O 4 samples. The synthesized products possess a specific capacitance of 1256 C/g at 1 A/g and an energy density of 69 Wh/kg at 1350 W/kg. Moreover, the assembled device retains 81% of its capacity after being fully charged and discharged 10,000 times.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
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IF 9.4
Wenxin Wang,Jiangjiang Zhang,Jinsheng Rong,Lanli Chen,Shiqiang Cui
Reducing the size of catalysts and tuning their electronic structure and interfacial properties are key to enhancing catalytic performance. Herein, a series of quantum-sized Co-based nanodot composites, including Co 3 O 4 /C, CoS 2 /C, CoN/C, and CoP/C, were synthesized using chemical vapor deposition (CVD) methods. By means of experimental measurement and theoretical calculation, CoP/C exhibited more robust electrochemical response than other Co-based compounds in electrochemical oxidation of N 2 H 4 (HzOR) and hydrogen evolution reaction (HER). The catalytic activities of CoP/C can be further enhanced by introducing Co vacancies on the surface of CoP/C (labeled as Co 1−x P/C). The results demonstrated that Co 1−x P/C not only exhibited notable electrochemical responses at an ultra-low N 2 H 4 concentration of 0.67 μM, showcasing its potential for ultra-sensitive N 2 H 4 detection but also realized HzOR instead of the oxygen evolution reaction (OER) half-reaction, thereby lowering the overpotential to 2.0 mV at 10.0 mA cm −2 . Finally, a Zn-hydrazine (Zn-Hz) battery was fabricated as a promising energy conversion device, showing the exceptional practical value of Co 1−x P/C.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Leyang Li,Ruiyang Sun,Rui Yuan,Manpeng Lin,Linlin Wang,Qi Wang,Jiguo Tu,Handong Jiao,Shuqiang Jiao
Molten-salt electrorefining (MSE) is currently the primary method for purifying many elements, offering promise for the sustainable upcycling of spent metals in the future. However, the conventional constant-current electrolysis protocol inevitably leads to deterioration of the microenvironment near the electrode, leading to reaction runaway and process inefficiency. In this work, we comprehensively studied for the first time the effect of constant- and pulse-electrolysis protocols on environmental evolution in electrode–electrolyte interfaces during the MSE of Ti, using a computer model. The results showed that compared to constant electrolysis, pulse-electrolysis protocols could effectively regulate the interfacial microenvironment and improve the electrorefining efficiency. Furthermore, a correlation between interfacial reconstruction and pulse parameters was established, indicating that the duty ratio was the key factor in inhibiting the deterioration of the interfacial microenvironment. To further verify the simulation results, the real-time morphological evolution of the electrodes during electrolysis was monitored by a novel in situ X-ray computed tomography (CT) technology under pulse-electrolysis protocols. The experimental results indicated that the pulse-electrolysis protocols enhanced the interfacial microenvironment and promoted electrolysis efficiency. Collectively, this work demonstrated that MSE could be effectively advanced by rationally designing the pulse-electrolysis protocols, facilitating its large-scale application in industry.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Zhuang Wang,Mian Li,Bin Fu,Wenping Cao,Xiangjie Bo
Although cobalt nitride (CoN)-based nanomaterials have been widely designed as advanced oxygen evolution reaction (OER), hydrogen evolution reaction (HER), and oxygen reduction reaction (ORR) catalysts, the continuous consumption of lithium-ion batteries (LIBs) has led to a high price of cobalt metal. Therefore, in the future, recycling valuable Co elements from spent devices and boosting their service efficiency will inevitably promote the utilization of Co-based materials in water splitting and zinc-air batteries (ZABs). Herein, we realize the Co recycling from spent LIBs by a simple hydrometallurgy method. Under the assistance of hexamethylenetetramine and polystyrene spheres, after the hydrothermal and pyrolysis treatment in the NH 3 atmosphere, the as-reclaimed cobalt oxalates were successfully transformed into novel three-dimensional (3D) CoN nanoflowers (denoted as CoN NFs). Benefiting from the unique 3D flower-like architectures, intrinsic high conductivity, large surface area, uniformly dispersed CoN nanoparticles, and the synergistic effect between Co 3 N and CoO phases, the 3D flower-like CoN NFs exhibited excellent OER catalytic activity. The performance was much better than commercial RuO 2 in the 1.0 M KOH solution. Furthermore, the CoN NFs-based water splitting cell needed a voltage of 1.608 V to achieve the current density of 10 mA cm −2 , which is even 16 mV smaller than that of Pt/C||RuO 2 benchmark (1.624 V). Meanwhile, the CoN NFs-derived ZAB exhibited a high peak power density of 107.3 mW cm −2 (vs. 103.2 mW cm −2 of Pt/C-RuO 2 -based ZAB) and a low charge–discharge voltage gap (0.93 V vs. 1.43 V of Pt/C-RuO 2 -based ZAB). Due to the excellent structural and elemental stabilities, the corresponding water splitting cell and ZAB had outstanding durability. This work successfully explored an advanced industrial chain from recycling Co metal in spent devices to designing the high-efficiency HER/OER/ORR electrocatalysts for advanced water splitting devices and ZABs. This will further promote the value-added utilization of valuable Co metal in various energy storage or conversion devices.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Bohao Kong,Hefeng Yuan,Zhehao Liu,Zizai Ma,Xiaoguang Wang
Engineering platinum-free catalysts for hydrogen evolution reaction (HER) with high activity and stability is essential for electrochemical hydrogen production . In this paper, we report the synthesis of cobalt-doped AlNi 3 /NiO (Co-AlNi 3 /NiO) electrode with three-dimensional nanoporous structure via chemical dealloying method. Density functional theory (DFT) calculations reveal that Co-AlNi 3 /NiO can accelerate water adsorption / dissociation and optimize adsorption–desorption energies of H* intermediates, thus improving the intrinsic HER activity. Both the introduction of Co and Al can efficiently ameliorate the electronic density around Ni sites of NiO and AlNi 3 , which can effectively reduce the energy barrier towards Volmer–Heyrovsky reaction and thus synergistically promote the hydrogen evolution. Benefiting from the large electrochemical active surface area , high electrical conductivity and electronic effect, the nanoporous Co-AlNi 3 /NiO catalyst exhibits remarkable HER activity with an overpotential of 73 mV at a current density of 10 mA cm −2 in alkaline condition, outperforming most of the reported non-precious metal catalysts . The nanoporous Co-AlNi 3 /NiO catalyst can operate continuously over 1000 h at high current densities with a robust stability. This work provides a new vision for the development of low-cost and efficient electrocatalysts for energy conversion applications.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhong Wang,Jinzhou Li,Shuang Yuan,Jinshuo Yang,Zhiqiang Jin,Xinjia Tan,Jie Dang,Wangzhong Mu,Guojian Li,Qiang Wang
FeCoNi-based high entropy intermetallic compounds are promising substitutes for noble metal catalysts for hydrogen evolution reaction (HER) and oxygen evolution (OER), while their activity is restricted by the synergistic effect between the elements. In this paper, the theoretical model of FeCoNiMnMoP bifunctional catalyst has been reasonably designed given the volcanic curve of M−H bond energy as a valuable guide for candidate metal elements. Theoretical calculations show that the synergistic effect between multiple sites not only accelerates the electron transfer but also reduces the rate-determining step (RDS) barrier. At the same time, the introduction of Mo also enhances the total density of states and reduces the d-band center, thus optimizing the adsorption and dissociation of intermediates. The experimental results confirm that the theoretical model has excellent catalytic performance. In the alkaline solution, FeCoNiMnMoP‖FeCoNiMnMoP requires only an ultra-low cell voltage of 1.49 V for overall water splitting when the current density is 10 mA cm −2 . In general, novel insights on the effects of intermetallic synergies on water decomposition are provided, which is helpful for the design of bifunctional catalysts based on volcanic diagrams.
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