JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Zhi-Qiang Hou,Wen-Ping Hu,Guo-Hua Yang,Zi-Xuan Zhang,Tian-Yi Cheng,Ke-Jing Huang
The production of high-purity hydrogen using surplus electrical energy and abundant water resources has immense potential in mitigating the fossil energy crisis, as hydrogen fuel holds clean, pollution-free, and high-energy characteristics. However, the practical application of large-scale hydrogen production from water faces challenges such as high overpotentials, sluggish dynamics, and limited electrocatalytic lifetime associated with the hydrogen evolution reaction (HER). Here, we fabricated the sandwich structure of a Ni/Fe 3 O 4 @poly(3,4-ethylene-dioxythiophene)/Ni (Ni/Fe 3 O 4 @PEDOT/Ni) electrode and employed a strong magnet to obtain a magnetic electrode capable of achieving high-activity and durability for HER. Electrochemical analysis reveals that the activated magnetic electrode displays a significantly reduced overpotential and an extended electrocatalytic lifetime of 10 days. Notably, its stability is higher than that of non-magnetic Ni/Fe 3 O 4 /Ni and Ni/Fe 3 O 4 @PEDOT/Ni electrodes, primarily due to the support from magnetic force and the protective PEDOT layer. Moreover, the minute atomized droplets can form the H 2 O 2 species in a moist environment, facilitating the formation of the NiO layer on the Ni surface, which plays a vital role in boosting catalytic activity. In conclusion, our magnetic electrode strategy, combined with the emergence of the NiO layer, offers valuable insights for the development of advanced HER electrodes.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
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IF 5.816
Bowen Lu,Yanhui Wang,Wei Li,Shiwei Song,Pengfei Tian,Rushuo Li,Xueqing Tian,Xiangyu Liu,Jianbing Zang
The development of self-supporting electrodes that exhibited both high efficiency and good durability remained a challenge in the field of hydrogen energy utilisation. Here, we designed a self-supporting 3D hierarchical porous electrode by filling carbon nanotubes (CNTs) loaded with Ni–P alloy into the framework of nickel foam (NF). Firstly, CNTs were decorated with a catalytically active Ni–P alloy via electroless plating (Ni–P@CNTs). Then, the Ni–P@CNTs were filled and anchored onto the framework of NF via electroplating to synthesise a self-supporting electrode (Ni–P@CNTs/NF). The Ni–P@CNTs/NF exhibited an excellent catalytic performance toward the hydrogen evolution reaction (HER) in 1 M KOH electrolyte, with an overpotential of 53 mV at 10 mA cm −2 , a small Tafel slope of 101.56 mV dec −1 and excellent long-term durability. This facile and effective strategy might provide a new path to the design of self-supporting electrodes with enhanced HER catalytic.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Zhuwei Yang,Linsen Li,Xiao Yang,Hui Xiong,Riguang Zhang,Zhao Jiang
In this study, a series of Ni-CeO 2 /TS-1 (Titanium Silicalite-1) catalysts were synthesized for dry reforming of methane (DRM). Among them, 5Ni-10CeO 2 /TS-1 exhibited the highest catalytic performance with 89 % CH 4 and 93 % CO 2 conversions, 4.81 mol CH4 ·g Ni -1 ·h −1 and 4.99 mol CO2 ·g Ni -1 ·h −1 specific activities, 95.5 % H 2 /CO ratio after 50 h, accompanied by the good stability with 2.9 % CH 4 and 2.3 % CO 2 activity loss within 100 h. Combined with various characterizations, the structure–function relationship was also investigated. For the physical and morphological analysis, it was indicated that the appropriate CeO 2 content could effectively diminish, disperse the Ni nanoparticles, and maintain MFI backbone structure. For the electronic structure, the introduced CeO 2 could improve the amount and strength of the surface Ni-O-X (Ti or Ce) species by changing the interaction among Ni nanoparticles, TS-1 and CeO 2 . It led to more Ni nanoparticles in stronger electron-deficient state, as well as more medium-strength basic sites, favoring for the activation of CH 4 and CO 2 . However, Ni nanoparticles would be covered when excessive CeO 2 was introduced, preventing the exposure of the active sites. Therefore, only the suitable CeO 2 in the catalysts could significantly improve catalytic performance for DRM with long-term stability. Furthermore, the good anti-sintering and anti-coking properties of 5Ni-10CeO 2 /TS-1 were mainly dependent on the optimal amount of surface Ni-O-X species with high strength. In-situ DRIFTS (diffuse reflectance infrared spectroscopy) analysis demonstrated that the introduced CeO 2 could help catalyst favor for activating CH 4 and CO 2 molecules, and inhibiting the CH 4 overcracking and carbon accumulation, confirmed by the long-term measurement and structure analysis of spent catalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Xiaoshuang Zhou,Bing Chen,Wei Wang,Liang Liu,Xiankai Li,Long Chen,Yanhui Li,Yanzhi Xia,Lijie Ci
The increasing requirements for wearable and portable electronics are driving the interests of high performance fiber supercapacitor. Layered double hydroxide (LDH) is broadly used in electrode materials, owing to the adjustability of components and the unique lamellar structure. However, limited active sites and poor electrical conductivity hinder its applications. Herein, the core–shell heterostructured Ni(OH) 2 @activation Zn-Co-Ni layered double hydroxides (Ni(OH) 2 @A-ZnCoNi-LDH) electrode was fabricated by loading pseudocapacitance material on the A-ZnCoNi-LDH to improve the electrochemical performance. Significantly, benefits from the synergistic effect of the multi-metal ions and the core–shell heterostructure, the electrodes demonstrated a capacitance of 2405 mF·cm −2 at 1 mA·cm −2 . Furthermore, Ni(OH) 2 @A-ZnCoNi-LDH was used as the core electrode and carbon nanotube (CNT) film coated with Fe 2 O 3 @reduced graphene oxide (rGO) was wrapped around the core electrode to assemble coaxial fiber asymmetric supercapacitor, which illustrated an ultrahigh energy density of 177.7 µWh·cm −2 at 0.75 mW·cm −2 . In particular, after consecutive charging and discharging 7000 cycles, the capacitance retention of the device was 95 %, indicating the excellent cycling stability. Furthermore, the device with high flexibility can be woven into textiles in different shapes. The fabricated device has an excellent development prospect as an energy source in wearable electronic devices.
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ACS Catalysis
·
2025
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IF 13.1
Shengpeng Mo,Shuangde Li,Jiangjing Zhou,Xin Zhao,Huimin Zhao,Xiaobin Zhou,Yinming Fan,Zongqiang Zhu,Bing Li,Qinglin Xie,Wenzhe Si,Yunfa Chen,Daiqi Ye,Junhua Li
A concentrated solar reaction device has been designed for the solar-driven photothermal CO2 reverse water–gas shift reaction, in which solar-to-chemical conversion efficiency would be up to 26% via a concentrated solar panel. Meanwhile, a special photothermal Ni–C–In catalyst (Ni/C–In2O3) with interstitial C, the In3Ni2 intermetallic compound, and disordered Ni clusters has been synthesized. As a result, the SO2-tolerant Ni/C–In2O3 catalyst exhibits an outstanding solar-driven photothermal catalytic performance (near thermodynamic limitation) with 100% CO selectivity and a 20.96 mmol gcat–1 h–1 CO production rate for solar-driven CO2 hydrogenation under concentrated solar irradiation (around 1521.9 mW/cm2) even sunlight without external heating. The incorporation of interstitial C and exposed Ni clusters in the Ni–C–In intermetallic catalyst could strengthen intensive solar light absorption. Moreover, quasi in situ XPS and DFT theoretical calculation results validate that asymmetric interaction between interstitial C and the Ni-cluster not only effectually regulates the electronic structure of the Ni–C–In intermetallic catalyst but also greatly optimizes the activation of H2 and CO2 molecules and the energy barriers of key reaction dynamics (HCOO* formation and dehydrogenation) in the RWGS reaction. Accordingly, this study provides a promising strategy for the electronic structure modification of photothermal functional catalysts with C modification to boost CO2 hydrogenation, putting forward an important step toward practical solar-to-fuel production with concentrated natural sunlight.
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Green Energy & Environment
·
2025
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IF 14.6
Conghao Ku,Lihua Du,Huidu Xu,Xucheng Li,Siyuan Long,Zhengli Liu,Ik Seon Kwon,Jeunghee Park,Weiran Yang
Selective total hydrogenation of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)tetrahydrofuran (BHMTHF) under mild condition is crucial in biomass refining, yet dauntingly challenging with non-precious metal catalysts. Herein, the hexagonal-close-packed (hcp) Ni dominated carbon-encapsulated Ni-based catalyst (Ni@C-3) was fabricated via a facile citric acid induced carbonization strategy, which exhibited an outstanding catalytic performance toward the hydrogenation of HMF, achieving a high BHMTHF yield of 95.4% under 70 °C and 2 MPa H 2 . Additionally, even at high HMF concentrations (2500 mM), it maintained an high BHMTHF yield of 89.7%. The carbon layer, derived from the thermal decomposition of citric acid, effectively prevents the agglomeration of Ni nanoparticles and suppresses the phase transition of hcp-Ni to fcc-Ni. The carbon-encapsulated structure ensures the excellent storage stability and reusability of catalysts. Structure-activity relationship studies demonstrated that the hcp-Ni (101) crystal facets effectively reduce the reaction energy barrier of the rate-determining step (furan ring hydrogenation) during the reaction process, thereby promoting the hydrogenation of HMF to BHMTHF. Furthermore, the Ni@C-3 exhibited excellent catalytic activity in the hydrogenation of compounds containing various functional groups. Notably, furfural can also be hydrogenated to tetrahydrofurfuryl alcohol (THFA) under solvent-free conditions, and the yield of THFA can reach 91.2%. This study provides a facile strategy for designing and developing advanced hydrogenation catalysts based on crystal phase engineering, which makes it a promising alternative to noble metal catalysts in biorefineries.
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ELECTROCHIMICA ACTA
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2018
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IF 5.116
Ze Chai,Chuanhai Jiang
The electrochemical/chemical growth of porous (Ni,Co,Cu)(OH) 2 was reported based on the corrosion behaviors of Ni-Co-Cu films in neutral salt spray . The films prepared by using electrodeposition were ternary solid solution alloys with a simple phase structure, strong texture, nanoscale grains, large microstrain and a large number of crystal defects . The unique microstructures coupled with extensive ion diffusion during the subsequent corrosion process facilitated the formation of ternary hydroxides with uniform and porous nanostructures . The ternary hydroxides composed of Ni-/Co-dominant hydrotalcite-like and Cu-dominant orthorhombic (Ni,Co,Cu)(OH) 2 could be efficiently prepared by motivating the transformation from oxide to hydroxide. The binder-free (Ni,Co,Cu)(OH) 2 electrode exhibited a high specific capacitance of 1738 F g −1 at a current density of 20 A g −1 and decent cycling stability. The electrochemical/chemical growth mode, uniform porous nanostructures and nature of the ternary hydroxides could account for the superior electrochemical performances. This work proposed a simple and green approach to prepare multicomponent hydroxides as novel electrode materials for rechargeable batteries and hybrid supercapacitors .
研究领域:
材料科学
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电化学
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储能技术
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纳米材料
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腐蚀科学
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INORGANIC CHEMISTRY
·
2023
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IF 4.6
Guangxin Ren,Baocang Liu,Liang Liu,Minghao Hu,Junpeng Zhu,Xuan Xu,Peng Jing,Jinfang Wu,Jun Zhang
Biomass is a sustainable and renewable resource that can be converted into valuable chemicals, reducing the demand for fossil energy. 5-Hydroxymethylfurfural (HMF), as an important biomass platform molecule, can be converted to high-value-added 2,5-furandicarboxylic acid (FDCA) via a green and renewable electrocatalytic oxidation route under mild reaction conditions, but efficient electrocatalysts are still lacking. Herein, we rationally fabricate a novel self-supported electrocatalyst of core–shell-structured copper hydroxide nanowires@cerium-doped nickel hydroxide nanosheets composite nanowires on a copper mesh (CuH_NWs@Ce:NiH_NSs/Cu) for electrocatalytically oxidizing HMF to FDCA. The integrated configuration of composite nanowires with rich interstitial spaces between them facilitates fast mass/electron transfer, improved conductivity, and complete exposure of active sites. The doping of Ce ions in nickel hydroxide nanosheets (NiH_NSs) and the coupling of copper hydroxide nanowires (CuH_NWs) regulate the electronic structure of the Ni active sites and optimize the adsorption strength of the active sites to the reactant, meanwhile promoting the generation of strong oxidation agents of Ni3+ species, thereby resulting in improved electrocatalytic activity. Consequently, the optimal CuH_NWs@Ce:NiH_NSs/Cu electrocatalyst is able to achieve a HMF conversion of 98.5% with a FDCA yield of 97.9% and a Faradaic efficiency of 98.0% at a low constant potential of 1.45 V versus reversible hydrogen electrode. Meanwhile, no activity attenuation can be found after 15 successive cycling tests. Such electrocatalytic performance suppresses most of the reported Cu-based and Ni-based electrocatalysts. This work highlights the importance of structure and doping engineering strategies for the rational fabrication of high-performance electrocatalysts for biomass upgrading.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Haibin Wang,Xiaoqiang Du,Xiaoshuang Zhang,Lu Li
Electrocatalytic water splitting has become one of the most promising and effective ways to solve energy crises and environmental pollution. In this work, a series of M-doped Co 3 O 4 materials with foreign ions (M = Ce, Ni and Fe) were grown on a Ni foam substrate through classical hydrothermal and calcination methods. It is worth noting that not all doping of foreign ions can promote the electrocatalytic performance of intrinsic materials. The Ce-doped Co 3 O 4 material shows excellent oxidation properties of water (overpotential of 320 mV at 50 mA cm −2 ) and urea (potential of 1.39 V at 50 mA cm −2 ). However, the doping of Ni reduces the water oxidation performance of the intrinsic material (overpotential of 410 mV@ 50 mA cm −2 ), and the doping of Fe reduces the urea oxidation performance of the inherent material (potential of 1.45 V@ 50 mA cm −2 ). A series of experimental results indicate that the improved activity of the Ce-Co 3 O 4 electrode is attributed to faster electron transport capacity, higher exposure to active sites, and improved conductivity due to doping of Ce. It is noteworthy that the doping of these ions does alter the rate-determination step for the water oxidation reaction. The stability test demonstrated that the current density of water oxidation and urea oxidation of the catalyst had no significant attenuation after a long electrocatalytic activity test. This work provides a new idea for improving the electrocatalytic activity of catalysts by a doping strategy.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Zekai Mu,Xianglei Liu,Hang Shi,Chao Song,Chunzhuo Dang,Ke Gao,Nan Sun,Cheng Tian,Hangbin Zheng,Xinrui Wang,Yimin Xuan
By converting two greenhouse gases into fuels, CO 2 reforming of CH 4 via free and clean solar energy is a promising solution to the energy shortage and global warming problems simultaneously. However, serious challenges such as limited light-to-fuel efficiency, severe catalyst aggregation, and deactivation still exist for reactors employing traditional catalyst powders. Here, Ni/MgAlO x -LDH catalysts loaded Ni foam reactor with heat recovery is proposed for highly efficient and stable CO 2 reforming under direct concentrated solar irradiation. The temperature nonuniformity is reduced by 84.3% compared to powdered systems, which benefits from the high thermal conductivity of nickel foams. Overheating is also prevented, which leads to much less carbon deposition and relieved active sites aggregation. Ultrahigh light-to-fuel efficiency of 36.51% is achieved, which is much higher than that of traditional powdered systems (23.87%). Numerical simulation results have an excellent agreement with experiments and demonstrate that heat recovery can greatly improve CRM rates by 23.8%. This work opens new routes to achieve highly efficient, stable, and scalable solar-driven CO 2 reforming via Ni/MgAlO x -LDH catalysts loaded Ni foam reactors with heat recovery.
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FUEL
·
2020
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IF 5.578
Limo He,Song Hu,Xiaofei Yin,Jun Xu,Hengda Han,Hanjian Li,Qiangqiang Ren,Sheng Su,Yi Wang,Jun Xiang
Fe-modified Ni/Al 2 O 3 catalysts with Fe/Ni molar ratios of 0, 0.5, 1 and 2 were prepared to promote the co-production of H 2 and carbon nanotubes (CNTs) during steam reforming of toluene as a tar model compound. After the addition of Fe, toluene conversion increased from 55.1% of Ni/Al 2 O 3 to 73.6% of F1N1A (Fe/Ni ratio of 1), and H 2 yield over F1N1A reached the maximum of more than 2000 mmol/(g-cata). Multi-walled carbon nanotubes with average diameter of 10–30 nm were generated and follow tip-growth mechanism. Compared with Ni/Al 2 O 3 , the addition of Fe remarkably increased the amount and quality of CNTs which had longer length and less tortuosity. These dual promoting effects on H 2 and CNTs after the addition of Fe were attributed to the strong interaction between Ni and Fe in Fe-Ni alloy. Fe-Ni alloy had the high activity for the decomposition performance of toluene and H 2 O to generate more H 2 and intermediates for improving the reforming reaction. Meanwhile, the high catalytic decomposition activity supplied more carbon species and the formation of Fe-Ni alloy enhanced the generation of metal carbide for promoting CNTs growth. Besides, the deposition of amorphous carbon was suppressed and the interaction between Ni particle and catalyst support was weakened after the addition of Fe, which kept the activity of catalyst and promoted the tip-growth of CNTs.
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CHEMOSPHERE
·
2019
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IF 5.108
Xin Ning,Yuhan Sun,Heyun Fu,Xiaolei Qu,Zhaoyi Xu,Shourong Zheng
Metal-organic frameworks (MOFs) have received significant attention as promising precursors or sacrificial templates in the preparation of porous carbon supported catalysts. In this study, N-doped porous carbon supported Ni catalysts (denoted as Ni/NC) were prepared using furfuryl alcohol (FA) loaded Ni-MOF-74 as the precursor followed by NH 4 OH treatment and pyrolysis under N 2 atmosphere. For comparison purpose, Ni catalysts supported on porous carbon (denoted as Ni/C) were also prepared by direct pyrolysis of Ni-MOF-74. The selective gas phase catalytic hydrodechlorination of 1,2-dichloroethane to ethylene was carried out to evaluate the catalytic performances of the catalysts. It was found that for Ni catalysts prepared at the same pyrolysis temperature, Ni particle sizes in Ni/NC catalysts were significantly smaller (20–40% smaller) than that of Ni/C. This reflected that pre-modification of Ni-MOF-74 using FA and NH 4 OH could effectively increase Ni dispersion in Ni catalysts derived from Ni-MOF-74. Moreover, Ni/NC had a markedly stronger ability to form spillover H 2 owing to the enhanced metal-support interactions by N-doping. Accordingly, Ni/NC catalysts exhibited much higher catalytic activities than Ni/C catalysts. The turnover frequencies of Ni/NC catalysts were found to be 1.22–1.65 times higher than Ni/C catalysts. Increasing pyrolysis temperature led to decreased catalytic activities of both Ni/C and Ni/NC catalysts, due to the aggregation of Ni particles at higher treatment temperature. The findings from this study demonstrate that the MOF-mediated synthesis method offers a promising way to prepare Ni-based catalysts for catalytic hydrodechlorination of chlorinated hydrocarbons .
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