MATERIALS SCIENCE AND ENGINEERING A-STRUCTURAL MATERIALS PROPERTIES MICROSTRUCTURE AND PROCESSING
·
2022
·
IF 6.044
Zeyun Cai,Tao Xiang,Weizong Bao,Jiayin Chen,Tian Gao,Guoqiang Xie
Pure titanium is an ideal material for tissue replacements and implant materials for its superior biocompatibility and corrosion resistance , but its limited strength remains a major obstacle to its wide applications. A promising strategy for enhancing the strength is to alloy the pure titanium with oxygen. Herein, we reported an oxygen solid solution strengthening for pure titanium by achieving a titanium-oxygen (Ti–O) alloy using ball milling (BM) and spark plasma sintering (SPS). The effect of oxygen contents, ranging from 0.33 to 2.08 wt%, on the mechanical properties of pure titanium was systematically investigated. Experimental results indicate that the Ti–O alloy with the oxygen content of 1.95 wt% reached an ultrahigh yield strength of 2026 MPa and showed a large ductility of 11.2% in compression. According to the quantified analysis of strengthening mechanisms, solid solute oxygen atoms are responsible for the balance of superior yield strength and ductility of the Ti–O alloys.
研究领域:
材料科学
·
生物医学工程
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产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2015
·Vol. 44
·期 19
·9182-9192
·
IF 4.197
Cholho Choe,Ling Yang,Zhanao Lv,Wanling Mo,Zhuqi Chen,Guangxin Li,Guochuan Yin
Redox-inactive metal ions can modulate the reactivity of redox-active metal ions in a variety of biological and chemical oxidations. Many synthetic models have been developed to help address the elusive roles of these redox-inactive metal ions. Using a non-heme manganese(II) complex as the model, the influence of redox-inactive metal ions as a Lewis acid on its catalytic efficiency in oxygen atom transfer was investigated. In the absence of redox-inactive metal ions, the manganese(II) catalyst is very sluggish, for example, in cyclooctene epoxidation, providing only 9.9% conversion with 4.1% yield of epoxide. However, addition of 2 equiv. of Al3+ to the manganese(II) catalyst sharply improves the epoxidation, providing up to 97.8% conversion with 91.4% yield of epoxide. EPR studies of the manganese(II) catalyst in the presence of an oxidant reveal a 16-line hyperfine structure centered at g = 2.0, clearly indicating the formation of a mixed valent di-μ-oxo-bridged diamond core, MnIII-(μ-O)2-MnIV. The presence of a Lewis acid like Al3+ causes the dissociation of this diamond MnIII-(μ-O)2-MnIV core to form monomeric manganese(IV) species which is responsible for improved epoxidation efficiency. This promotional effect has also been observed in other manganese complexes bearing various non-heme ligands. The findings presented here have provided a promising strategy to explore the catalytic reactivity of some di-μ-oxo-bridged complexes by adding non-redox metal ions to in situ dissociate those dimeric cores and may also provide clues to understand the mechanism of methane monooxygenase which has a similar diiron diamond core as the intermediate.
研究领域:
生物化学
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催化化学
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产品关联
DOI
PubMed
高影响因子
Journal of Physical Chemistry C
·
2021
·
IF 4.126
Lu Zhang,Guojun Yuan,Xinyu Wang,Jianliang Bai,Yaqing Zhu,Lili Ren
Environmental pressure gives potential for the application of transition metal phosphides (TMPs), which serve as efficient degradation catalysts. Although various efforts are advocated to obtain high activity, it is still difficult for phosphides to exhibit cycle performance in hydrodechlorination (HDC), limiting their practical development. By linking the changes in the oxidation state of MoP before and after HDC with its catalytic performance, the Mo–P–O bond is found to be the active catalytic site, not only promoting electron transfer but also forming the defect-rich structure. Based on this, H2O2-treated MoP after HDC reached a performance of 19.9%, and the activity could be restored after multiple cycle reactions, while the untreated one still had poor performance, demonstrating that carrying out the H2O2 treatment process can realize the recycling of MoP, which is of importance for industrial application of catalysts.
研究领域:
化学
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环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF PORPHYRINS AND PHTHALOCYANINES
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2016
·Vol. 19
·期 12
·1238-1250
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IF 1.087
Mian HR Mahmood,Hua-Hua Wang,Hai-Yang Liu,Chi-Kwong Chang
Seven A 3 - and trans -A 2 B manganese(III) corroles ( 1–7- Mn) differing widely in their electronic and steric features were synthesized and transformed to their corresponding β -brominated manganese(III) corroles derivatives ( 1a–7a- Mn). Their corresponding (oxo)manganese(V) corroles 1–7- Mn(oxo) and 1a–7a- Mn(oxo) were further prepapred by treating with iodosylbenzene (PhIO). The reactivity for the oxygen atom transfer from 1–7- Mn(oxo) to styrene followed the order of 1- Mn(oxo) > 2- Mn(oxo) > 7- Mn(oxo) > 4- Mn(oxo) > 3- Mn(oxo) > 6- Mn(oxo) ≈ 5- Mn(oxo). The same pattern was observed for their β -brominated analogs 1a–7a- Mn(oxo), albeit their reactivity was remarkably higher. The steric protection of Mn V ≡ O moiety by ortho – ortho ′-dibromophenyl substituents was found to enhance the stability of (oxo)manganese(V) corroles significantly.
研究领域:
化学
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材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Lingfei Luo,Huimin Yang,Xiang Li,Kechen Zhou,Lu Tang,Huiyu Su,Liyan Chen,Chaofan Ma,Xiaoxia Wang,Dawen Zeng
The inert gas adsorption of outer oxygen atoms is becoming an important factor limiting the gas sensing activity of two-dimensional MoO 3 nanoflowers, which makes it necessary to modify the surface activity of MoO 3 nanoflowers. For a long time, the unique activity of Co atoms has attracted much attention in gas sensing. In this work, Co metal sites were introduced into MoO 3 defective nanoflowers (MoO 3 DNFs) by doping, which further improved the H 2 S gas sensing performance of MoO 3 DNFs. Based on H 2 S gas sensing experiment, the relationship between Co doping amount and gas sensing performance was constructed, and the optimal Co doping ratio was obtained. Finally, the adsorption reaction process of H 2 S gas molecules on MoO 3 -Co DNFs was simulated by DFT calculation, and the activation effect of Co metal sites on outer oxygen atoms was revealed.
研究领域:
材料科学
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传感器技术
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表面化学
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纳米结构材料
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气体检测
✓ 已验证
DOI
高影响因子
DALTON TRANSACTIONS
·
2016
·Vol. 45
·期 28
·11369-11383
·
IF 4.177
Zhanao Lv,Wenrui Zheng,Zhuqi Chen,Zhiming Tang,Wanling Mo,Guochuan Yin
Non-redox metal ions can affect the reactivity of active redox metal ions in versatile biological and heterogeneous oxidation processes; however, the intrinsic roles of these non-redox ions still remain elusive. This work demonstrates the first example of the use of non-redox metal ions as Lewis acids to sharply improve the catalytic oxygen atom transfer efficiency of a ruthenium complex bearing the classic 2,2′-bipyridine ligand. In the absence of Lewis acid, the oxidation of ruthenium(II) complex by PhI(OAc)2 generates the Ru(IV)O species, which is very sluggish for olefin epoxidation. When Ru(bpy)2Cl2 was tested as a catalyst alone, only 21.2% of cyclooctene was converted, and the yield of 1,2-epoxycyclooctane was only 6.7%. As evidenced by electronic absorption spectra and EPR studies, both the oxidation of Ru(II) by PhI(OAc)2 and the reduction of Ru(IV)O by olefin are kinetically slow. However, adding non-redox metal ions such as Al(III) can sharply improve the oxygen transfer efficiency of the catalyst to 100% conversion with 89.9% yield of epoxide under identical conditions. Through various spectroscopic characterizations, an adduct of Ru(IV)O with Al(III), Ru(IV)O/Al(III), was proposed to serve as the active species for epoxidation, which in turn generated a Ru(III)–O–Ru(III) dimer as the reduced form. In particular, both the oxygen transfer from Ru(IV)O/Al(III) to olefin and the oxidation of Ru(III)–O–Ru(III) back to the active Ru(IV)O/Al(III) species in the catalytic cycle can be remarkably accelerated by adding a non-redox metal, such as Al(III). These results have important implications for the role played by non-redox metal ions in catalytic oxidation at redox metal centers as well as for the understanding of the redox mechanism of ruthenium catalysts in the oxygen atom transfer reaction.
研究领域:
催化化学
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配位化学
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有机合成
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DOI
高影响因子
WATER RESEARCH
·
2023
·
IF 12.8
Jialiang Liang,Jingke Wu,Pengfei Gan,Yudan Liu,Peng Zhen,Yunyi Li,Zhiwei Zhao,Wen Liu,Meiping Tong
Organophosphorus pesticides are extensively utilized worldwide, but their incomplete dephosphorization poses significant environmental risks. This study investigates the dephosphorization of dimethoate (DMT), a representative organophosphorus pesticide, using a vacuum ultraviolet system. Surprisingly, in addition to hydroxyl radicals ( • OH), non-radical processes such as photoexcitation and singlet oxygen atoms (O( 1 D)) exert more significant effects on DMT dephosphorization. The degradation kinetics of DMT demonstrate a perfect linear correlation with the radical yield in both UV-based and VUV-based advanced oxidation processes (AOPs), with greater efficacy of radical attack observed in the VUV system. This heightened efficiency is attributed to the excitation of DMT to a high-energy excited state induced by UV 185 radiation. Additionally, • OH alone is inadequate for achieving complete dephosphorization of DMT. The Fukui index and singly occupied orbital (SOMO) analysis reveal that the O( 1 D) generated by UV 185 -induced photolysis of O 2 exhibits exceptional selectivity towards P=S bonds, thereby playing an indispensable role in the dephosphorization process of DMT. This study highlights the significant contribution of non-radical pathways in DMT dephosphorization by VUV, which holds great implications for the advancement of photochemical-based AOPs.
研究领域:
环境科学
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农药化学
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产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 56
·期 1
·364-379
·
IF 3.553
Huo Hang,Jiang Yanqiu,Wang Zhe,Hu Yanjing,Zhao Tingting,Liu Xing,Xu Xianzhu,Lin Kaifeng
Abstract In this paper, urea group functionalized periodic mesoporous organosilica was utilized as matrix to introduce cobalt precursor into framework. After pyrolysis in nitrogen atmosphere, urea group was decomposed into carbon species and simultaneously the cobalt precursor was reduced to metallic cobalt nanoparticles. The metallic cobalt nanoparticles can be stabilized by coordinating to carbonyl oxygen atoms in carbon species. The supported metallic cobalt exhibited excellent catalytic performance towards 4-nitrophenol hydrogenation reaction. The largest turnover frequency number can reach up to 164.8 h −1 , and the reaction rate constant can be as high as 0.77 min −1 . The influence of pyrolysis temperature on catalytic performance was also investigated. Compared with the results obtained by samples prepared with wet impregnation method or different pyrolysis rate, it can be concluded that the coordination to carbonyl oxygen atom in carbon species plays a crucial role in improving electron transfer between metallic cobalt and carbon species during catalytic procedure. Graphic abstract Metallic cobalt nanoparticles with high dispersion were introduced into urea group functionalized mesoporous silica matrix via pyrolysis in nitrogen atmosphere. The coordination to carbonyl oxygen atom enhances the catalytic performance in 4-nitrophenol hydrogenation.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-9
·
IF 16.6
Gao Xiaofeng,Zhu Ling,Yang Feng,Zhang Lei,Xu Wenhao,Zhou Xian,Huang Yongkang,Song Houhong,Lin Lili,Wen Xiaodong,Ma Ding,Yao Siyu
Oxidative dehydrogenation of propane is a promising technology for the preparation of propene. Boron-based nonmetal catalysts exhibit remarkable selectivity toward propene and limit the generation of CO x byproducts due to unique radical-mediated C–H activation. However, due to the high barrier of O-H bond cleavage in the presence of O 2 , the radical initialization of the B-based materials requires a high temperature to proceed, which decreases the thermodynamic advantages of the oxidative dehydrogenation reaction. Here, we report that the boron oxide overlayer formed in situ over metallic Ni nanoparticles exhibits extraordinarily low-temperature activity and selectivity for the ODHP reaction. With the assistance of subsurface Ni, the surface specific activity of the BO x overlayer reaches 93 times higher than that of bare boron nitride. A mechanistic study reveals that the strong affinity of the subsurface Ni to the oxygen atoms reduces the barrier of radical initiation and thereby balances the rates of the BO-H cleavage and the regeneration of boron hydroxyl groups, accounting for the excellent low-temperature performance of Ni@BO x /BN catalysts.
研究领域:
催化
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Fiber Materials
·
2023
·
IF 16.1
Fu Xiaohan,Wang Juan,Qian Dejian,Xi Linhe,Chen Liang,Du Yawei,Cui Wenguo,Wang Yan
Cellular respiration can provide energy for wound healing. However, some of retarded healing processes in local hyperglycemic environment suffer from a decrease in cellular adaptation to oxygen, thus reducing in situ oxidative metabolism. Herein, a three-dimensional (3D) extracellular matrix (ECM) bionic short fibrous sponge was prepared for chronic diabetic wound healing and effectively regulated cellular respiration by enhancing cellular adaptation to oxygen and remolding the local tissue microenvironment. The 3D bionic sponge scaffold exhibited good cell adhesion, biocompatibility, bioactivity, and, most importantly, aggregated oxygen atoms on the graphene oxide (GO) surface. In an in vitro assay, the oxygen atom-concentrating short fibrous sponge activated monocyte chemoattractant protein-1 (MCP-1), induced the expression of vascular endothelial growth factor (VEGF), and effectively promoted angiogenesis in a hyperglycemic environment. The sponge was also applied to diabetic wounds in vivo to verify its roles in the promotion of angiogenesis and collagen deposition. These experiments confirmed the synergistic effect of GO with adipose-derived stem cells (ADSCs), which could further promote diabetic wound healing. Therefore, oxygen atom-concentrating short fibrous sponges that regulate cellular respiration provide a new idea for the repair of poorly healing wounds by improving oxidative metabolism and have importantclinical significance. Graphical abstract The oxygen-rich characteristics of short fibrous sponges with aggregational oxygen atoms can optimize the water absorption performance of short fibers, effectively regulate cell respiration and improve tissue oxidation metabolism by improving the ability of cells to adapt to oxygen, and provide important application value for tissue damage repair in collaboration with ADSCs.
研究领域:
生物医学工程
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组织工程
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材料科学
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再生医学
✓ 已验证
产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2018
·Vol. 5
·期 6
·1391-1396
·
IF 5.106
Gulbahar Dawut,Yong Lu,Licheng Miao,Jun Chen
We report high-performance aqueous Zn-ion batteries consisting of a zinc anode, a poly(benzoquinonyl sulfide) (PBQS) cathode, and a 3 M Zn(CF3SO3)2 aqueous electrolyte. The PBQS cathode displays an initial discharge capacity of 203 mA h g−1 at 0.1C and a good capacity retention of 86% after 50 cycles at 0.2C. The PBQS cathode can deliver a high reversible capacity of 126 mA h g−1 at a high rate of 5.0C. Meanwhile, we also studied the redox mechanism during discharge/charge processes by ex situ infrared spectra and theoretical calculations, revealing that reversible bonding of Zn2+ ions with carbonyl oxygen atoms in PBQS occurs in the redox reactions of PBQS molecules. The redox reactions of PBQS molecules can be regarded as the reversible bonding of Zn2+ ions with carbonyl oxygen atoms in PBQS.
研究领域:
材料科学
·
电化学
·
能量存储
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ying Xu,Genkuo Nie,Xiao Jiang,Hongyu Wang,Guihua Yang,Ziyi Yan,Ji-Jun Zou,Hailong Yu,Shitao Yu,Yu Liu
Metal-metal oxide catalysts are robust in selective hydrodeoxygenation of biomass derives. Herein, 1-hexanol in total yield about 76 % is firstly achieved by high selective hydrodeoxygenation of 5-hydroxymethylfurfural over Ni/MCM-41 and Pt-WO X /t-ZrO 2 . By controlling the amount ratio of Ni/Ni 2+ to 0.46, a 99.9 % yield of 2,5-tetrahydrofurandimethanol was achieved from 5-hydroxymethylfurfural by Ni/MCM-41. Subsequently high yield of 76 % of 1-hexanol was obtained by competing pathways of tandem reactions beginning at SN2 reaction at the epoxy atom of 2,5-tetrahydrofurandimethanol to enol/tautomer intermediates and ending with controllable selective hydrogenation. The reaction mechanism is explored and the reaction-oriented regulation is realized by the additional strong BrÖnsted acid sites generated by electron transfer from W to Pt and the appropriate amount of Pt 0 sites of Pt-WO X /t-ZrO 2 , where the ratios of W 5+ /W 6+ and Pt 0 /Pt 2+ are 0.31 and 4.58 respectively. This work provides a new and green method for the synthesis of 1-hexanol and expands the utilization of metal–metal oxide in making value-added products using sustainable feedstocks.
研究领域:
催化
·
化学工程
·
绿色化学
·
生物质转化
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）