MATERIALS CHEMISTRY AND PHYSICS
·
2024
·
IF 4.3
Shufei Li,Shujun Qiu,Yong Shen Chua,Yongpeng Xia,Yongjin Zou,Fen Xu,Lixian Sun,Hailiang Chu
Rapid release of hydrogen at ambient condition is highly favorable and is necessary for fuel cell power generation on-demand. Hydrolysis of hydrides offers such advantage with sodium borohydride (NaBH 4 ) as a representative exemplar. Despite with exceptionally high hydrogen content, the hydrolysis kinetics of NaBH 4 is sluggish in the absence of catalyst. Co–B alloy has generally been employed as effective catalyst in the hydrolysis of borohydrides. However, Co–B particles are prone to agglomeration during the reaction, reducing the activity and durability of the catalyst. In this work, waxberry-like hierarchical porous carbon microspheres (HPCMs) were successfully prepared and were used as carriers to support Co–B particles to form the Co–B/HPCMs catalyst. The effects of HPCMs with different nitrogen contents in Co–B/HPCMs on the catalytic dehydrogenation rate of NaBH 4 hydrolysis were systematically investigated. The experimental results showed that Co–B/HPCM-2 exhibited excellent catalytic activity in the hydrolysis of NaBH 4 at 298 K, with a low activation energy of 43.3 kJ ·mol −1 and a high hydrogen generation rate of 3083.1 ml H2 ·min −1 ·g −1 . Moreover, after five consecutive cycles, its catalytic activity maintained at 91.7 % of the initial catalytic activity, displaying satisfactory cycling performance. The findings obtained from this study are expected to expand a novel path for the development of efficient Co-based catalysts in heterogeneous catalytic reactions .
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 7
·070539
·
IF 4.316
Runyue Qin,Yunpeng Pan,Zeang Duan,Huanhuan Su,Kailiang Ren,Wenfeng Wang,Yuan Li,Ning Xi,Yu Wang,Lu Zhang,Shumin Han
Nickel layered double hydroxide, Ni(OH)2, has been widely used as the cathode for nickel based battery systems. However, the currently commercialized β-Ni(OH)2 is limited by its low capacity. In contrast, α-Ni(OH)2 can give higher capacity, but it is challenging to stabilize in alkaline solution due to the conversion to β-Ni(OH)2. Herein, we use zinc doped Ni(OH)2 and control its spherical morphology to strengthen the stability of α-Ni(OH)2 in a nickel metal hydride battery system. With an optimal zinc doping content of 3 mol% for the spherical α-Ni(OH)2 (Ni-Zn3), the cathode shows the highest discharge capacity of 351.3 mAh g–1 at a current density of 70 mA g–1 (0.2 C) and superior rate performance, which even delivers 271.5 mAh g–1 at 5 C. More importantly, the durability of the Ni-Zn3 cathode is significantly enhanced, which maintains 81.7% after cycling 360 times, almost twice as long as that of pure α-Ni(OH)2. Studies show that the stabilized Ni–O bond and suitable aperture structure are mainly responsible for the advanced electrochemical properties of the Ni-Zn3. The results show that proper zinc doping spherical α-Ni(OH)2 with low-cost and high performance is an promising cathode material for nickel-based battery systems.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Binbin Jin,Xin Ye,Heng Zhong,Fangming Jin
Efficient conversion of CO2/bicarbonate into chemicals using solar energy as driving force is meaningful to alleviate global warming caused by excessive CO2 emission. In this work, a direct light-driven method of bicarbonate hydrogenation into formate over a nanocatalyst Pd/TiO2 is proposed. Formic acid has recently attracted increasing attention as a promising hydrogen storage carrier. By using the Pd/TiO2, the reaction system achieved a self-heating effect under irradiation, promoting the hydrogenation of bicarbonate. Owing to its extraordinary photothermal conversion ability and efficient light utilization, the 5 wt % Pd/TiO2 exhibited a high photothermal conversion efficiency of 30.9% under experimental illumination. The desirable performance of the Pd/TiO2 catalyst for hydrogenation of bicarbonate is attributed to the elevated temperature from the localized surface plasmon resonance effect of nano-Pd and the direct participation of photogenerated carriers in hydrogenation of bicarbonate. This study combined the merits of photocatalysis and thermocatalysis, providing a promising method for light-driven conversion of CO2 using the photothermal synergistic effect.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Senliang Xi,Xiaojun Wang,Kudzaishe Caren Tome,Tonghuan Zhang,Zongying Han,Meng Gao,Shixue Zhou,Hao Yu
The hydrogen storage performances of MgH 2 improved by the addition of Ni and SAPO-34 were studied in detail. The mixture of MgH 2 with Ni and SAPO-34 was a physical reaction as shown by the X-ray diffraction (XRD) results. The SAPO-34 and Ni were uniformly distributed on the surface of MgH 2 . The thermodynamic and kinetic properties of 90MgH 2 /5Ni/5SAPO-34 were investigated by differential scanning calorimetry (DSC) and pressure-composition-isothermal (PCI) methods. The results showed that the dehydrogenation activation energy of 90MgH 2 /5Ni/5SAPO-34 decreased by 64.3 kJ/mol compared with that of MgH 2 . In addition, the relationship between the value of dehydrogenation heat and hydrogen content was also investigated by in-situ calorimetry. The enthalpy value of each sample in the dehydrogenation processes were calculated by in-situ calorimetry measurement. The dehydrogenation enthalpies of as-milled MgH 2 and 90MgH 2 /5Ni/5SAPO-34 were 63.2 kJ/mol H 2 and 53.6 kJ/mol H 2 , respectively. Thus, the co-doping of Ni and SAPO-34 contributed significantly to decrease the thermodynamic stability and improve the hydrogen sorption kinetic properties of MgH 2 .
研究领域:
材料科学
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氢储能技术
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物理化学
✓ 已验证
DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 22
·15547-15554
·
IF 3.3
Changyin Zhong,Yifei Yang,Yun Fang,Jun Chen,Bomin Feng,Hongbing Wang,Wenhua Luo,Yunxi Yao
Lanthanum oxide (La2O3) possesses superior reactivity during catalytic hydrogenation, but the intrinsic activity of La2O3 toward H2 adsorption and activation remains unclear. In the present work, we fundamentally investigated hydrogen interaction with Ni-modified La2O3. Hydrogen temperature programmed desorption (H2-TPD) on Ni/La2O3 shows enhanced hydrogen adsorption with a new hydrogen desorption peak at a higher temperature position compared to that on the metallic Ni surfaces. By systematically exploring the desorption experiments, the enhanced H2 adsorption on Ni/La2O3 is due to the oxygen vacancies formed at the metal–oxide interfaces. Hydrogen atoms transfer from Ni surfaces to the oxygen vacancies to form lanthanum oxyhydride species (H–La–O) at the metal–oxide interfaces. The adsorbed hydrogen at the metal–oxide interfaces of Ni/La2O3 results in improved catalytic reactivity in CO2 methanation. Furthermore, the enhanced hydrogen adsorption on the interfacial oxygen vacancies is ubiquitous for La2O3-supported Fe, Co, and Ni nanoparticles. Benefiting from the modification effect of the supported transition metal nanoparticles, the surface oxyhydride species can be formed on La2O3 surfaces, which resembles the recently reported oxyhydride observed on the reducible CeO2 surfaces with abundant surface oxygen vacancies. These findings strengthen our understanding of the surface chemistry of La2O3 and shed new light on the design of highly efficient La2O3-based catalysts with metal–oxide interfaces.
研究领域:
催化
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表面化学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Chao Ma,Baozhou Zhao,Jianguang Yuan,Yunfeng Zhu,Jiguang Zhang,Bogu Liu,Ying Wu,Liquan Li,Shaoxiong Zhou
Herein, nanodisc-like MnTiO 3 was successfully prepared via a hydrothermal method , and for the first time, the MnTiO 3 nanodiscs were doped into magnesium hydride (MgH 2 ) for the study. In the first dehydrogenation cycle, MgH 2 -8 wt% MnTiO 3 showed a low onset hydrogen release temperature of 202 °C, while MnTiO 3 was transformed into Mg 6 MnO 8 and TiO x by reaction with MgH 2 , which played a real catalyst in the subsequent reaction. The composite system could instantly absorb 4.79 wt% H 2 in 100 s at 150 °C and rapidly release about 5.71 wt% H 2 in 500 s at 300 °C. The Kissinger plot revealed that the dehydrogenation activation energy dropped to 72.06 kJ/mol, which was significantly lower than that of as-milled MgH 2 . Moreover, after 50 isothermal cycles, the composite system still has an excellent capacity retention rate of 94.4 %. Compositional and structural analysis indicated that the in situ formation of TiO x and Mg 6 MnO 8 during dehydrogenation provided a multivalent multielement catalytic surrounding that accelerated the H atoms adsorption and dissociation, yielding a better kinetic property of MgH 2 .
研究领域:
材料科学
·
能源存储
·
催化
✓ 已验证
DOI
高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2023
·
IF 4.3
Xinya Yao,Ying Li,Yuetian Guo,Keli Zhong,Lijun Tang,Xiaomei Yan
Reversible detection of bisulfite (HSO 3 - ) and hydrogen peroxide (H 2 O 2 ) is highly desirable in biology and food safety owing to their redox pair function in biological systems and their utilization in food industry. In this work, a ratiometric fluorescent probe ( TPA-Y ) with aggregation-induced emission (AIE) properties based on triphenylamine fluorophore was designed and synthesized for reversibly monitoring of HSO 3 - /H 2 O 2 . Reaction of HSO 3 - with TPA-Y can result in ratiometric fluorescence changes ( I 444 / I 629 ), and the emission spectrum blue shift reaches 185 nm, which can effectively avoid spectral overlap. Meanwhile, the solution color changed obviously from orange to colorless, enabling naked eye detection of HSO 3 - . TPA-Y was capable of quantitatively detect HSO 3 - in sugar and wine samples with the recovery rates ranging from 94.52 to 102.18%. In addition, TPA-Y is suitable to prepare paper strips and anti-counterfeiting ink for HSO 3 - detection. In addition, the original TPA-Y can be released after the addition product ( TPA-Y-HSO 3 - ) is oxidized by H 2 O 2 , and the HSO 3 - /H 2 O 2 redox cycle can repeat for at least six times. The probe TPA-Y can be applied to fluorescence imaging of reversible and dynamic interconversion between HSO 3 - and H 2 O 2 in living MCF-7 cells.
研究领域:
生物化学
·
食品安全
·
分析化学
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Yang Zeng,Lan Jiang,Xiaoxin Zhang,Songhai Xie,Yan Pei,Gongbing Zhou,Weiming Hua,Minghua Qiao,Zhen-Hua Li,Baoning Zong
Catalytic hydrogenolysis of biomass-derived glycerol to 1,3-propanediol (1,3-PDO) represents an important process for the sustainable production of value-added chemicals. However, there is a dearth of understanding of the effect of the polymorph of the support on this reaction. Herein, two Pt–WOx/TiO2 catalysts supported on rutile TiO2 (r-TiO2) and anatase TiO2 (a-TiO2) polymorphs were prepared to investigate the crystal phase effect of TiO2 on the structural property and catalytic performance in glycerol hydrogenolysis. The TiO2 polymorph was identified to impose profound effects on the size of the Pt nanoparticles (NPs) and the dispersion and location of the WOx species, which originated from the discrepancies in the crystal structures between the PtO2 and the TiO2 polymorphs and the discrepancies in the interactions of WOx with different TiO2 polymorphs. In glycerol hydrogenolysis, the Pt–WOx/r-TiO2 catalyst gave a 1,3-PDO selectivity of 51.2% at a glycerol conversion to liquid products of 74.5%, yielding 38.1% of 1,3-PDO. In contrast, the Pt–WOx/a-TiO2 catalyst showed much inferior glycerol conversion and 1,3-PDO selectivity, yielding only 1.0% of 1,3-PDO under identical reaction conditions. The superior catalytic performance of the Pt–WOx/r-TiO2 catalyst is attributed to the r-TiO2 polymorph that facilitates a faster hydrogen spillover than the a-TiO2 polymorph from the Pt NPs to the reaction intermediate on the WOx species, which is substantiated by an even higher 1,3-PDO yield of 44.8% over the physically mixed Pt/r-TiO2 + WOx/r-TiO2 catalyst. This work demonstrates the critical role of the polymorph of the TiO2 support in the design of efficacious Pt–WOx-based catalysts for glycerol hydrogenolysis to 1,3-PDO.
研究领域:
催化化学
·
材料科学
·
可再生能源
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Liuting Zhang,Ze Sun,Zeliang Cai,Nianhua Yan,Xiong Lu,Xinqiao Zhu,Lixin Chen
Transition metal nanoparticles have shown great catalytic effect on MgH 2 , yet excellent cyclic stability can be attached due to the addition of carbon nanotubes. In this paper, MgH 2 + 10 wt% Zr 0.4 Ti 0.6 Co /5 wt% Carbon nanotubes (CNTs) composite is designed to investigate the synergistic modification of Zr 0.4 Ti 0.6 Co nanosheets and carbon nanotubes on the hydrogen storage performance of MgH 2 . Compared with pure MgH 2 , the initial hydrogen release temperature of MgH 2 + 10 wt% Zr 0.4 Ti 0.6 Co /5 wt% CNTs composite decreases to 180 °C and the composite can quickly release 90% H 2 within 10 min at 300 °C. In addition, the completely dehydrogenated sample can absorb 3.51 wt% H 2 within 20 min under 3 Mpa hydrogen pressure at 125 °C. Ulteriorly, the activation energy values of dehydrogenation and rehydrogenation of MgH 2 decrease to 70.5 ± 7.8 kJ/mol and 35.8 ± 3.8 kJ/mol on account of the presence of 10 wt% Zr 0.4 Ti 0.6 Co/5 wt% CNTs , which reasonably explains the remarkable reduction of the temperature for hydrogen sorption. Furthermore, the MgH 2 + 10 wt% Zr 0.4 Ti 0.6 Co /5 wt% CNTs composite shows excellent cycling performance, indicative of potential application in practical hydrogen storage in the nearest future.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Kejun Shi,Shu Xiao,Qingdong Ruan,Hao Wu,Guohua Chen,Chilou Zhou,Saihua Jiang,Ke Xi,Mohan He,Paul K. Chu
A method for in situ deposition of multi-layered graphene (MLG) coatings is demonstrated to mitigate hydrogen embrittlement of the X70 pipe steel. Carbon is implanted into the nickel catalytic layer pre-deposited by electroplating on the surface of the pipe steel, followed by annealing to segregate and form MLG. The MLG coatings are investigated systematically with respect to the surface morphology, phase structure, hydrogen resistance, corrosion resistance, and molecular dynamics simulation. In the stacked MLG structure, the in situ grown graphene layers interpenetrate each other to boost the coating adhesion and hydrogen resistance. Diffusion and the solid solution formed between the Ni coating and substrate improve the adhesion strength after annealing. The diffusion coefficient and permeability are reduced by 123 times and 48 times, respectively. Slow strain rate tests demonstrate outstanding resistance against hydrogen embrittlement because the MLG coatings inhibit hydrogen evolution, extend the diffusion path, decrease the permeation area, and enhance hydrogen adsorption. Moreover, electrochemical tests indicate that the MLG coatings have better corrosion resistance. These results reveal a viable strategy to use graphene to protect commercial steels from hydrogen embrittlement.
研究领域:
材料科学
·
工程学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Yu Gu,Haijun Liu,Miaomiao Yang,Zhipeng Ma,Lianming Zhao,Wei Xing,Pingping Wu,Xinmei Liu,Svetlana Mintova,Peng Bai,Zifeng Yan
The relatively low cost and mild toxicity of vanadium makes it an alternative to commercially applied Pt and Cr based catalysts in propane dehydrogenation (PDH). Conventional VO x /Al 2 O 3 catalyst shows high initial activity, but deactivates fast due to severe coke formation, which requires frequent regeneration by coke combustion and causes massive CO 2 emissions. In this context, we report on the phosphine (PH 3 ) surface modification of VO x /Al 2 O 3 catalyst leading to substantial improvement of its stability. The phosphorus considerably modifies the properties of the VO x /Al 2 O 3 catalyst: (i) tunes surface acidity, (ii) separates polymerized vanadium oxide species and (iii) weakens interaction between vanadium species with alumina support. Synergy among all these factors facilitates desorption of produced propylene and inhibit the oligomerization of coke precursors, which contributed to the enhancement of the catalyst stability during propane dehydrogenation.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
DOI
高影响因子
Journal of Cleaner Production
·
2021
·
IF 9.297
Tong Wen,Yunliang Zhao,Xiangke Jiao,Guang Yang,Zixuan Zhang,Wei Wang,Tingting Zhang,Qiwu Zhang,Shaoxian Song
The use of sediment wastes after water treatment , from traditional wastewater management to secondary resource recycling, has attracted increasing attention. In this work, the feasibility, catalytic effect and mechanism of using artificial copper-based precipitation as photo-Fenton-like catalysts were investaged. According to the XRD , SEM-EDS, XPS and various photoelectric characterizations, the copper-based precipitation showed the potential acting as a photo-Fenton-like catalyst due to its abundant copper ions and photoresponse characteristics. The 0.06 g L −1 copper-based precipitation decolors 97% of methylene blue with initial concentration of 20 mg L −1 within 20 min assisted by H 2 O 2 and light, which is superior to the commonly used catalysts in terms of decolorization rate and catalysts dosage. Excellent catalytic performance is by virtue of the enhanced reduction reaction from Cu(II) to Cu(I), resulting in an increasing utilization rate of hydrogen peroxide, and increasing ·OH for decoloration. In addition, the catalyst activity can be replicated in successive experiments without a significant decline, further suggesting the feasibility from wastes to materials. The research progress shows the potential value of secondary resources containing posnjakite based on its unique character.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）