Small
·
2025
·
IF 12.1
Shaojian Jiang,Yuhang Liu,Ruidong Yang,Lijun Zhang,Wenke Liu,Kai Deng,Hongjie Yu,Hongjing Wang,Liang Wang
Since formaldehyde oxidation reaction (FOR) can release H 2 , it is attractive to construct a bipolar hydrogen production system consisting of FOR and hydrogen evolution reaction (HER). Although copper-based catalysts have attracted much attention due to their low cost and high FOR activity, the performance enhancement mechanism lacks in-depth investigation. Here, an amorphous-crystalline catalyst of amorphous nickel hydroxide-coated copper dendrites on copper foam (Cu@Ni(OH) 2 /CF) is prepared. The modification of Ni(OH) 2 resulted in hydrophilic and aerophobic states on the Cu@Ni(OH) 2 /CF surface, facilitating the transport of liquid-phase species on the electrode surface and accelerating the release of H 2 . The Open circuit potential (OCP) and density functional theory (DFT) calculations indicate that this core–shell structure facilitates the adsorption of HCHO and OH − . In addition, the catalytic mechanism and reaction pathway of FOR are investigated through in situ FTIR and DFT calculations, and the results showed that the modification of Ni(OH) 2 lowered the energy barrier for C─H bond breaking and H─H bond formation. In the HER//FOR system, Pt/C//Cu@Ni(OH) 2 /CF can provide a current density of 0.5 A cm −2 at 0.36 V and achieve efficient and stable H 2 production. This work offers new ideas for designing electrocatalysts for bipolar hydrogen production system assisted with formaldehyde oxidation.
研究领域:
电化学
·
催化材料
·
能源转换与存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2019
·
IF 5.04
Zhewen Ma,Jianxin Zou,Darvaish Khan,Wen Zhu,Chuanzhu Hu,Xiaoqin Zeng,Wenjiang Ding
Two kinds of metal-organic frameworks (MOFs) based on Co (II) and Fe (II) as metal ions and trimasic acid (TMA) as organic linker were synthesized. They were used to prepare corresponding MgH 2 -TM MOF (TM = Co, Fe) composites via ball-milling. X-ray diffraction analyses show the formation of Mg 2 Co and α-Fe phases in MgH 2 -TM MOF composites after decomposition. Both of the well dispersed Mg 2 Co and α-Fe nanoparticles exhibit considerable catalytic efficiency in accelerating the sorption kinetics of MgH 2 . The dehydrogenated MgH 2 -Fe MOF composite shows faster hydriding kinetics than the pure MgH 2 and MgH 2 -Co MOF. Meanwhile, the apparent dehydrogenation activation energy ( E d ) of the MgH 2 -Co MOF and MgH 2 -Fe MOF composites are 151.3 ± 9.4 and 142.3 ± 6.5 kJ/mol H 2 , both of which are lower than that of pure MgH 2 (181.4 ± 9.2 kJ/mol H 2 ). The improvement on the sorption kinetics of the MgH 2 -TM MOF powders is mainly attributed to the catalytic effects of nano-sized Mg 2 Co and α-Fe formed on the surface of Mg/MgH 2 particles.
研究领域:
材料科学
·
能源储存
✓ 已验证
DOI
高影响因子
Materials Today Nano
·
2021
·
IF 8.109
B. Liu,B. Zhang,X. Chen,Y. Lv,H. Huang,J. Yuan,W. Lv,Y. Wu
Transition metals are the traditional catalysts to improve the hydrogen storage performance of Mg. In the present article, the multi-valence Co catalyst (Co@CNTs) is prepared to improve the kinetics of Mg. The dehydrogenation temperature decreases, and desorption kinetics of MgH 2 is significantly enhanced by the addition of the catalyst. The dehydrogenation of MgH 2 –Co@CNTs composite is a random bulk nucleation/surface and three-dimensional growth with constant interface velocity reaction. Although the dehydrogenation activation energy of MgH 2 –Co@CNTs composite is reduced, the enthalpy change and entropy change of the composite are similar to the raw MgH 2 , which means the dehydrogenation is mainly dissociation of MgH 2 . Besides, the cycle performance of MgH 2 –Co@CNTs composite is stable. The damping of the performance for the composite is negligible after 50 cycles, which benefits from the in-site formed Co 3 MgC 0.5 in the composite. The Co 3 MgC 0.5 can act as a ‘hydrogen pump’ to adjust the hydrogen storage performance of Mg. Theoretical studies show that multi-valence Co can trap H 2 molecules and weaken their σ-bonds. In the first cycle, the bridging effect of Co plays an important role in the improvement of H 2 dissociation and release. In the subsequent cycles, Co 6 C 1 becomes the active site to assist the hydrogenation and dehydrogenation of the composite.
研究领域:
材料科学
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能源存储
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 24
·14629-14637
·
IF 10.733
Chong Lu,Yanling Ma,Fan Li,Hong Zhu,Xiaoqin Zeng,Wenjiang Ding,Tao Deng,Jianbo Wu,Jianxin Zou
A core–shell nanostructured Mg@Pt composite, consisting many of icosahedral Mg particles as the core with nano-sized Pt particles distributed homogeneously on different surfaces, was synthesized through an arc plasma method followed by the generic solid-state method. The microstructures and hydrogen sorption properties of the Mg@Pt composite were carefully investigated and compared to that of pure Mg powder. In particular, the dehydrogenation behaviors of the hydrogenated Mg@Pt composite were observed in situ via high-resolution transmission electron microscopy (HRTEM). The results revealed that the Pt on Mg particles showed a “spillover” effect to improve the hydrogen absorption kinetics in the early stage. It then transformed into H-stabilized Mg3Pt, followed by the formation of MgH2. DFT calculation and in situ TEM observations demonstrated that the H-stabilized Mg3Pt acted as a “hydrogen pump” for the dehydrogenation of MgH2 and then transformed into Pt after desorption. Through this effect, the dehydriding kinetics of the hydrogenated Mg@Pt composite was improved and the onset dehydrogenation temperature was reduced compared to that of the pure MgH2 powder.
研究领域:
材料科学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Girma Sisay,Hairus Abdullah,Dong-Hau Kuo,Worku Lakew,Hardy Shuwanto,Sleshi Fentie
The works on photocatalytic hydrogen production and green chemical conversion have received significant attention due to the current need for clean energy and a secure environment. Herein, Ce and Ga codoped Zn(O,S) has been synthesized with different amounts of Ce using facile precipitation method at a low temperature of 95 °C and characterized by XRD, SEM, HRTEM, XPS, EPR, Raman, DRS, PL, EIS, UV–vis, GC–MS, and photocurrent response measurements. The as-prepared photocatalysts were utilized for hydrogen production and hydrogenation of toxic organic compounds, viz. nitrobenzene (NB) and azobenzene (AB) into a valuable product of aniline. The incorporation of Ce and Ga into Zn(O,S) enhanced the hydrogen evolution and hydrogenation reactions of NB and AB. This notable enhancement was ascribed to the synergistic effects of Ce and Ga dopants to form positively charged defects that trap the photogenerated electron. The trapping mechanism improves the photogenerated charge separation and transfer as confirmed with impedance spectroscopy (EIS), transient photocurrent response, and PL measurements. The highest hydrogen production was attained by 15Ce-5Ga-Zn(O,S) with a rate of 7130 μmol∙g − 1 ∙h − 1 in 10% ethanol solution. In addition, NB and AB were effectively converted to aniline in 15 min and 30 min, respectively. A plausible photocatalytic hydrogenation mechanism for both hydrogenation of NB and AB is proposed with the steps of surface adsorption, molecular diffusion, pinning at oxygen vacancy sites, and hydrogenation reaction with the help of in situ generated H + coupled with electrons.
研究领域:
材料科学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Xiao Chen,Wenqi Liu,Jingjie Luo,Hongyu Niu,Rongrong Li,Changhai Liang
The hydrogenation of furfural containing multifunctional group often needs the high-efficiency cooperation of multiple catalytic active centers, which is greatly determined by the regulation of the surface and interface structure of multicomponent catalytic materials. Based on such circumstance, a series of highly dispersed supported bimetallic Cu–Ni catalysts prepared by the in situ topological transformation of layered double hydroxides have been investigated for the one-pot hydrogenation of furfural. Compared with the supported monometallic Cu and Ni catalysts, the optimized bimetallic Cu1Ni3/MgAlO catalyst presents highly efficient and good selectivity in the hydrogenation of furfural at the bath reactor. The selectivity to tetrahydrofurfuryl alcohol reaches 94.0% with a complete conversion of furfural at 110 °C under 3 MPa of H2 for 3 h. The results of TEM and in situ FT-IR confirm that the Ni-rich Cu–Ni alloy in the Cu1Ni3/MgAlO catalyst generates a strong synergistic effect, which shifts the adsorption configuration of furfural from parallel or vertical adsorption to tilted adsorption so as to significantly improve the catalytic performance. The intrinsic catalytic performances of CuxNiy/MgAlO catalysts indicate that the TOFC═O and TOFC═C values can be balanced through construction of the structure of the catalyst for achieving the synergistic effect between Cu and Ni significantly to enhance the one-pot selective hydrogenation of furfural to tetrahydrofurfuryl alcohol. Additionally, the Cu1Ni3/MgAlO catalyst presents excellent reusability by six-cycle testing. The above results indicate that the Cu1Ni3/MgAlO with the cooperation of multiple catalytic active centers is a promising catalyst for the selective hydrogenation of furfural.
研究领域:
催化化学
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材料科学
·
可再生资源转化
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2022
·
IF 10.319
Yang Zhao,Tong Li,Haixiang Huang,Tingting Xu,Bogu Liu,Bao Zhang,Jianguang Yuan,Ying Wu
MgH 2 has a high theoretical hydrogen production capacity and mild conditions for hydrogen production by hydrolysis, so it is suitable as an ideal hydrogen source for fuel cells. However, with the progress of the hydrolysis reaction, MgH 2 is impeded from reacting further by the continuous deposition of magnesium hydroxide on its surface, resulting in low hydrogen yield and slow reaction kinetics. In the present work, a highly efficient NiCo bimetallic synergistic catalysis is developed to improve the hydrolysis performance of MgH 2 . The MgH 2 -8 wt% NiCo@C composite ball-milled for 5 h achieves nearly 100% hydrogen desorption efficiency within 15 min in 0.05 mol L –1 MgCl 2 solution. Because the interaction between Ni and Co on the surface of MgH 2 can form a channel for rapid hydrogen evolution, which hinders the continuous formation of the Mg(OH) 2 passivation layer and promotes the hydrolysis reaction of MgH 2 . This is very important for the implementation of MgH 2 hydrolysis to produce hydrogen in the future.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Magnesium and Alloys
·
2021
·
IF 10.088
Shun Wang,Mingxia Gao,Zhihao Yao,Kaicheng Xian,Meihong Wu,Yongfeng Liu,Wenping Sun,Hongge Pan
Magnesium hydride (MgH 2 ) is one of the most promising hydrogen storage materials for practical application due to its favorable reversibility, low cost and environmental benign; however, it suffers from high dehydrogenation temperature and slow sorption kinetics. Exploring proper catalysts with high and sustainable activity is extremely desired for substantially improving the hydrogen storage properties of MgH 2 . In this work, a composite catalyst with high-loading of ultrafine Ni nanoparticles (NPs) uniformly dispersed on porous hollow carbon nanospheres is developed, which shows superior catalytic activity towards the de-/hydrogenation of MgH 2 . With an addition of 5 wt% of the composite, which contains 90 wt% Ni NPs, the onset and peak dehydrogenation temperatures of MgH 2 are lowered to 190 and 242 °C, respectively. 6.2 wt% H 2 is rapidly released within 30 min at 250 °C. The amount of H 2 that the dehydrogenation product can absorb at a low temperature of 150 °C in only 250 s is very close to the initial dehydrogenation value. A dehydrogenation capacity of 6.4 wt% remains after 50 cycles at a moderate cyclic regime, corresponding to a capacity retention of 94.1%. The Ni NPs are highly active, reacting with MgH 2 and forming nanosized Mg 2 Ni/Mg 2 NiH 4 . They act as catalysts during hydrogen sorption cycling, and maintain a high dispersibility with the help of the dispersive role of the carbon substrate, leading to sustainably catalytic activity. The present work provides new insight into designing stable and highly active catalysts for promoting the (de)hydrogenation kinetics of MgH 2 .
研究领域:
材料科学
·
催化
·
储氢
·
纳米技术
✓ 已验证
DOI
高影响因子
Journal of Energy Storage
·
2023
·
IF 9.4
Weitao Shi,Feifan Hong,Renhuan Li,Ruolin Zhao,Sizhi Ding,Ziqi Liu,Peilin Qing,Yi Fan,Haizhen Liu,Jin Guo,Zhiqiang Lan
MgH 2 is a promising high-capacity solid hydrogen storage material. In this work, MnO 2 -doped Ti 3 C 2 (Ti 3 C 2 @MnO 2 ) was synthesized and used as a catalyst to improve the hydrogen storage performance of MgH 2 . We found that the dehydrogenated 10 wt% Ti 3 C 2 @MnO 2 -doped MgH 2 sample exhibited good hydrogen adsorption ability even at room temperature (30 °C), and could absorb 5.13 wt% of hydrogen in 400 s at 75 °C. The re‑hydrogenated Ti 3 C 2 @MnO 2 -doped MgH 2 sample started to release hydrogen at 182 °C and required 484 s to completely release hydrogen at 275 °C with a dehydrogenation capacity of 6.4 wt%. The Ti 3 C 2 @MnO 2 composite did not change the thermodynamic properties of MgH 2 . In the MgH 2 + Ti 3 C 2 @MnO 2 sample, Ti 3 C 2 , TiO 2 , MnO 2 , MnO, and Mn combined with MgH 2 to form Ti 3 C 2 /MgH 2 , TiO 2 /MgH 2 , MnO 2 /MgH 2 , MnO/MgH 2 , and Mn/MgH 2 multiphase interfaces, which improved the hydrogen storage performance of MgH 2 . The findings of this work may provide a new strategy for preparing novel and efficient catalysts for hydrogen storage applications.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
Small
·
2024
·Vol. 21
·期 1
·2406022
·
IF 13
Jiamin Zhao,Meimei Kou,Qing Yuan,Ying Yuan,Jinsheng Zhao
Tungsten carbide (WC x ) is a promising alternative to platinum catalysts for hydrogen evolution reaction (HER). However, strong tungsten–hydrogen bond hinders hydrogen desorption while favoring H + reduction, thus limiting HER kinetics. Inspired by the phenomenon of hydrogen spillover in heterogeneous catalysis, a ruthenium (Ru) doped-driven activated hydrogen migration from WC x surface to Ru is reported. This approach achieved high activity with an ultralow overpotential of 9.0 mV at 10 mA·cm −2 and superior stability at an industrial-grade current density of 1.0 A·cm −2 @ 1.65 V. In situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) and operando electrochemical impedance spectra revealed that this exceptional hydrogen production—which surpasses that of previously reported Pt/C catalysts—is attributable to the outstanding ability of WC x to induce water dissociation and hydrogen spillover from WC x to Ru surface. During the HER process, the rigid interfacial water network negatively affected the HER efficiency under alkaline conditions. The WC x sites disrupted this rigid structure, facilitating the contact between activated hydrogen (H * ) and WC x sites. Subsequently, H * migrates to Ru surface, where hydrogen recombination occurs to produce H 2 . This work paves a new avenue for the construction of coupled catalysts at the atomic scale to facilitate HER electrocatalysis.
研究领域:
电化学
·
催化材料
·
能源科学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2024
·
IF 10.7
Shuaipeng Wang,Shengli Zhu,Zhenduo Cui,Zhaoyang Li,Shuilin Wu,Wence Xu,Zhonghui Gao,Yanqin Liang,Hui Jiang
The quest for a cost-effective, high-performance catalyst for hydrogen production from electrolyzed water across a broad pH range holds immense importance. B, N co-doped Mo2C was first synthesized via microwave plasma chemical vapor deposition (MPCVD) for efficient hydrogen production from electrolyzed water. The B, N-Mo2C catalyst demonstrates a requirement of 81 mV in 1.0 M KOH to achieve a current density of 10 mA cm−2. Density functional theory (DFT) calculations revealed that B, N co-doping optimizes the charge transfer between H* and Mo2C, diminishes the excessive hydrogen binding energy of Mo2C, and supports effective and stable hydrogen evolution reaction (HER) conduction in diverse settings. This doping strategy offers a systematic design approach for designing highly active noble-metal-free HER catalysts.
研究领域:
材料科学
·
理论计算化学
✓ 已验证
产品关联
DOI
高影响因子
Energy Material Advances
·
2023
·
IF 12.9
Haixiang Huang,Jinting Chen,Tingting Xu,Yujie Lv,Bogu Liu,Bao Zhang,Jianguang Yuan,Ying Wu
Complex metal oxide catalysts greatly accelerate the hydrogen sorption rates in the magnesium hydride system. In this study, the graphene-supported Sc2O3/TiO2 catalyst is synthesized by means of a simple method, and a surprisingly synergetic effect of the Sc2O3-TiO2 cocatalyst on the hydrogen storage performance of MgH2 is observed. The MgH2-Sc2O3/TiO2@Gn composite starts to release hydrogen at 140 °C and reaches the peak dehydrogenation temperature at 239.9 °C. It absorbs 6.55 wt% of H2 in 1 min and desorbs 5.71 wt% of H2 in 10 min at 300 °C, showing excellent hydrogen absorption and desorption performance. Furthermore, with the decrease of the grain size and changes in the structure, the activity of the catalyst is greatly improved. The low-valent titanium and scandium and oxygen vacancies formed in the process of dehydrogenation facilitate hydrogen diffusion and electron transfer, and further improve the kinetic performance of the Mg/MgH2-Sc2O3/TiO2@Gn system. This study aims to provide insights into studying complex metal oxides as catalysts to improve hydrogen storage performance, and shed light on other catalysis-related research.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
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