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Article ; Online: Elimination of grain boundary resistance in vanadoborate electrolyte

Zhang, Shan / Lu, Ying / Sun, Xiu-Wei / Tian, Hong-Rui / Bai, Xue / Liu, Shu-Xia

Chemical communications (Cambridge, England)

2023 Volume 59, Issue 29, Page(s) 4312–4315

Abstract: An effective method to eliminate grain boundary resistance of crystalline vanadoborate electrolyte was developed. This method involved the addition of glycerol to result in the formation of many hydrogen bonds between crystal grains, facilitating a rapid ...

Abstract	An effective method to eliminate grain boundary resistance of crystalline vanadoborate electrolyte was developed. This method involved the addition of glycerol to result in the formation of many hydrogen bonds between crystal grains, facilitating a rapid transfer of protons across grain boundaries. Using this method, the intrinsic conduction of vanadoborate electrolyte was fully reflected in its bulk materials, valuable for advancing our understanding of vanadoborate electrolytes and for promoting the application of these electrolytes.
Language	English
Publishing date	2023-04-06
Publishing country	England
Document type	Journal Article
ZDB-ID	1472881-3
ISSN	1364-548X ; 1359-7345 ; 0009-241X
ISSN (online)	1364-548X
ISSN	1359-7345 ; 0009-241X
DOI	10.1039/d3cc00404j
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Highly efficient multi-site synergistic catalysis of a polyoxovanadate-based metal–organic framework for benzylic C–H bond oxidation

Dang, Tian-Yi / Li, Run-Han / Tian, Hong-Rui / Guan, Wei / Lu, Ying / Liu, Shu-Xia

Journal of materials chemistry A. 2022 Aug. 10, v. 10, no. 31

2022

Abstract: The selective oxidation of C–H bonds of benzylic compounds to synthesize high-value-added ketones remains a challenge under mild conditions, and the ambiguity of its oxidation mechanism limits the further development of this field. In this work, we ... ...

Abstract	The selective oxidation of C–H bonds of benzylic compounds to synthesize high-value-added ketones remains a challenge under mild conditions, and the ambiguity of its oxidation mechanism limits the further development of this field. In this work, we construct a polyoxometalate-based metal–organic framework (POMOF), [CuI2Cuᴵᴵ(bix)₂]{V₄O₁₂} (1, bix = 1,4-bis(imidazole-1-ylmethyl)benzene), successfully achieving the efficient oxidation catalysis of various benzylic compounds with outstanding conversion, selectivity and durability under mild conditions. Our experimental studies suggest that the highly catalytic activity of 1 derives from its attractive structure with multiple active sites, which consists of Vⱽ centers in a unique U-type {V₄O₁₂}⁴⁻ ({V₄}) cluster and Cuᴵ and Cuᴵᴵ centers bridged to the {V₄} cluster. Importantly, further theoretical calculations indicate that there exists synergistic catalysis between Cuᴵ/{V₄} sites and Cuᴵᴵ/{V₄} sites for 1 as catalyst in the oxidation of benzylic compounds, where the {V₄} cluster mainly provides deprotonation and oxidation sites, and the Cuᴵ site plays a role in the reduction of the oxidant, while the Cuᴵᴵ site plays a role in the adsorption of the oxidant. This is the first POMOF whose catalytic mechanism towards the oxidation of benzylic C–H bonds is deeply studied through the combination of experiments and theoretical calculations, providing a new perspective for the design of related catalysts.
Keywords	adsorption ; catalysts ; catalytic activity ; coordination polymers ; deprotonation ; durability ; oxidants ; oxidation
Language	English
Dates of publication	2022-0810
Size	p. 16514-16523.
Publishing place	The Royal Society of Chemistry
Document type	Article
ZDB-ID	2702232-8
ISSN	2050-7496 ; 2050-7488
ISSN (online)	2050-7496
ISSN	2050-7488
DOI	10.1039/d2ta03886b
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Hollow Lindqvist-like-Shaped {V

Tian, Hong-Rui / Zhang, Zhong / Dang, Tian-Yi / Liu, Shu-Mei / Lu, Ying / Liu, Shu-Xia

Inorganic chemistry

2021 Volume 60, Issue 2, Page(s) 840–845

Abstract: A polyoxovanadate-based nickel-organic framework, [Ni(bib) ...

Abstract	A polyoxovanadate-based nickel-organic framework, [Ni(bib)
Language	English
Publishing date	2021-01-06
Publishing country	United States
Document type	Journal Article
ZDB-ID	1484438-2
ISSN	1520-510X ; 0020-1669
ISSN (online)	1520-510X
ISSN	0020-1669
DOI	10.1021/acs.inorgchem.0c02890
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Article ; Online: A novel polyoxovanadate-based Co-MOF: highly efficient and selective oxidation of a mustard gas simulant by two-site synergetic catalysis

Tian, Hong-Rui / Zhang, Zhong / Liu, Shumei / Dang, Tian-Yi / Li, Xiao-Hui / Lü, Ying / Liu, Shu-Xia

Journal of materials chemistry A. 2020 June 30, v. 8, no. 25 p.12398-12405

2020

Abstract: Two novel polyoxovanadate-based metal–organic frameworks (MOFs), [Co(bib)]{V₂O₆} (V–Co-MOF) and [Ni(en)(bib)]{V₂O₆}·2H₂O (V–Ni-MOF) (bib = 1,4-bis(1H-imidazoly-1-yl)benzene, en = ethylenediamine) were facilely synthesized under mild hydrothermal ... ...

Abstract	Two novel polyoxovanadate-based metal–organic frameworks (MOFs), [Co(bib)]{V₂O₆} (V–Co-MOF) and [Ni(en)(bib)]{V₂O₆}·2H₂O (V–Ni-MOF) (bib = 1,4-bis(1H-imidazoly-1-yl)benzene, en = ethylenediamine) were facilely synthesized under mild hydrothermal conditions. Single-crystal X-ray diffraction analysis shows that the V sites in both compounds adopt {VO₄} tetrahedral coordination geometries, and the Co center in the V–Co-MOF presents a four-coordinated distorted tetrahedron configuration (coordinatively unsaturated metal sites, CUMS), while the Ni center in the V–Ni-MOF exhibits six-coordinated octahedral geometry (coordinatively saturated metal sites, CSMS). Given that the CUMS can generally be used as active sites for catalytic reactions, we explored the catalytic activities of these two compounds for the oxidation of a mustard gas simulant, 2-chloroethyl ethyl sulfide (CEES). The experimental results indicate that they can catalyze the oxidation of CEES to give the only nontoxic product, 2-chloroethyl ethyl sulfoxide (CEESO). Significantly, the V–Co-MOF exhibits higher catalytic activity; it converts 100% of CEES in 10 min, whereas V–Ni-MOF converts only 47.5% of CEES under identical conditions. Researching the mechanism of the catalytic reaction revealed that the excellent catalytic performance of the V–Co-MOF was attributed to the two-site synergetic effect: (1) the oxidant H₂O₂ interacts with the V site to produce peroxovanadium with higher oxidation activity; (2) the S atom in CEES coordinates with the four-coordinated Co(ii) center to obtain 2-chloroethyl ethyl sulfonium cation (CEES+), which makes the CEES more easily oxidize to CEESO based on the oxidation mechanism of peroxovanadium and shortens the molecular size distance between CEES and the obtained peroxovanadium, thereby greatly improving the rate of the catalytic reaction. To our knowledge, this is the first dual-active-site polyoxometalate-based MOF catalyst for catalysing the oxidative detoxification of CEES.
Keywords	X-ray diffraction ; active sites ; aromatic compounds ; catalysts ; catalytic activity ; cations ; cobalt ; coordination polymers ; ethylenediamines ; geometry ; hydrogen peroxide ; molecular weight ; nickel ; organic sulfur compounds ; oxidants ; oxidation
Language	English
Dates of publication	2020-0630
Size	p. 12398-12405.
Publishing place	The Royal Society of Chemistry
Document type	Article ; Online
ZDB-ID	2702232-8
ISSN	2050-7496 ; 2050-7488
ISSN (online)	2050-7496
ISSN	2050-7488
DOI	10.1039/d0ta00537a
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Article ; Online: A highly stable polyoxovanadate-based Cu(i)–MOF for the carboxylative cyclization of CO₂ with propargylic alcohols at room temperature

Tian, Hong-Rui / Zhang, Zhong / Liu, Shumei / Dang, Tian-Yi / Li, Zhuo / Lü, Ying / Liu, Shu-Xia

Green chemistry. 2020 Nov. 2, v. 22, no. 21 p.7513-7520

2020

Abstract: A novel polyoxovanadate-based copper(i)–organic framework, [Cuᴵ(bib)]₄{Vⱽ₄O₁₂} (V–Cu–MOF, bib = 1,4-bis(1H-imidazoly-1-yl)benzene), is facilely synthesized under mild hydrothermal conditions. The structure of the V–Cu–MOF is constructed from a cyclic {V₄ ... ...

Abstract	A novel polyoxovanadate-based copper(i)–organic framework, [Cuᴵ(bib)]₄{Vⱽ₄O₁₂} (V–Cu–MOF, bib = 1,4-bis(1H-imidazoly-1-yl)benzene), is facilely synthesized under mild hydrothermal conditions. The structure of the V–Cu–MOF is constructed from a cyclic {V₄O₁₂}⁴⁻ polyanion cluster and a 1D chain Cu(i)–MOF ([Cuᴵ(bib)]⁺). The presence of the {V₄O₁₂}⁴⁻ cluster stabilizes the Cu(i)–MOF with Cu(i) as the center, thereby improving the stability of the V–Cu–MOF and enabling it to stably exist in various solvents and pH = 2–12 solutions. Additionally, the V–Cu–MOF as a heterogeneous catalyst can catalyze the carboxylative cyclization of CO₂ and propargylic alcohols to high value-added α-alkylidene cyclic carbonates at room temperature, and the conversion and selectivity are almost 100%. More importantly, no obvious decrease in the yield of the α-alkylidene cyclic carbonate is observed after ten cycles. These results indicate the excellent catalytic activity and sustainability of the V–Cu–MOF. Research on the mechanism of the catalytic reaction suggests that the high-density Cu(i) sites in the V–Cu–MOF are the catalytically active centers for activating the CC bonds of propargylic alcohols. To the best of our knowledge, this is the first example of polyoxometalate-based metal–organic framework catalyst for catalyzing the conversion of CO₂ to value-added α-alkylidene cyclic carbonates at room temperature.
Keywords	ambient temperature ; anions ; carbon dioxide ; carbonates ; catalysts ; catalytic activity ; coordination polymers ; copper ; green chemistry ; pH ; value added
Language	English
Dates of publication	2020-1102
Size	p. 7513-7520.
Publishing place	The Royal Society of Chemistry
Document type	Article ; Online
Note	NAL-AP-2-clean
ZDB-ID	2006274-6
ISSN	1463-9270 ; 1463-9262
ISSN (online)	1463-9270
ISSN	1463-9262
DOI	10.1039/d0gc02812f
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: A universal strategy for fabrication and morphology control of polyoxometalate-based metal–organic frameworks

Li, Xiao-Hui / Liu, Yi-Wei / Lü, Ying / Zhang, Zhong / Tian, Hong-Rui / Liu, Shumei / Liu, Shu-Xia

Chemical communications. 2020 Feb. 6, v. 56, no. 11 p.1641-1644

2020

Abstract: A novel method is proposed to fabricate polyoxometalate-based metal–organic frameworks (POM@MOFs) by using the ability of POMs to oxidize metals to cations. The morphology-controlled growth of POM@MOFs (NENU-nNENU-n are a series of crystalline compounds ... ...

Abstract	A novel method is proposed to fabricate polyoxometalate-based metal–organic frameworks (POM@MOFs) by using the ability of POMs to oxidize metals to cations. The morphology-controlled growth of POM@MOFs (NENU-nNENU-n are a series of crystalline compounds constructed by a series of Keggin-type POMs encapsulated in a scaffold of Cu₃(BTC)₂, formulated as [Cu₁₂(BTC)₈(H₂O)₁₂][HₙXVₓM₁₂₋ₓO₄₀] (X = Si, Ge, P, As; M = W, Mo; x = 0, 1, 2, 3).) is achieved in the absence of any modulators and an effect of polyoxoanion charge number on morphology is observed.
Keywords	arsenic ; cations ; chemical reactions ; coordination polymers ; encapsulation ; germanium ; molybdenum ; silicon
Language	English
Dates of publication	2020-0206
Size	p. 1641-1644.
Publishing place	The Royal Society of Chemistry
Document type	Article ; Online
ZDB-ID	1472881-3
ISSN	1364-548X ; 1359-7345 ; 0009-241X
ISSN (online)	1364-548X
ISSN	1359-7345 ; 0009-241X
DOI	10.1039/c9cc09554c
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Article ; Online: A fast and highly selective Congo red adsorption material based on a cadmium-phosphonate network.

Ai, Jing / Tian, Hong-Rui / Min, Xue / Wang, Zi-Chuan / Sun, Zhong-Ming

Dalton transactions (Cambridge, England : 2003)

2019 Volume 49, Issue 12, Page(s) 3700–3705

Abstract: In this work, a cadmium-phosphonate network was prepared based on a tetrahedral shaped tetraphosphonic acid linker. The resulting three-dimensional compound ... ...

Abstract	In this work, a cadmium-phosphonate network was prepared based on a tetrahedral shaped tetraphosphonic acid linker. The resulting three-dimensional compound Cd
Language	English
Publishing date	2019-06-19
Publishing country	England
Document type	Journal Article
ZDB-ID	1472887-4
ISSN	1477-9234 ; 1364-5447 ; 0300-9246 ; 1477-9226
ISSN (online)	1477-9234 ; 1364-5447
ISSN	0300-9246 ; 1477-9226
DOI	10.1039/c9dt01545k
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: A universal strategy for fabrication and morphology control of polyoxometalate-based metal-organic frameworks.

Li, Xiao-Hui / Liu, Yi-Wei / Lu, Ying / Zhang, Zhong / Tian, Hong-Rui / Liu, Shu-Mei / Liu, Shu-Xia

Chemical communications (Cambridge, England)

2020 Volume 56, Issue 11, Page(s) 1641–1644

Abstract: A novel method is proposed to fabricate polyoxometalate-based metal-organic frameworks (POM@MOFs) by using the ability of POMs to oxidize metals to cations. The morphology-controlled growth of POM@MOFs (NENU-n) is achieved in the absence of any ... ...

Abstract	A novel method is proposed to fabricate polyoxometalate-based metal-organic frameworks (POM@MOFs) by using the ability of POMs to oxidize metals to cations. The morphology-controlled growth of POM@MOFs (NENU-n) is achieved in the absence of any modulators and an effect of polyoxoanion charge number on morphology is observed.
Language	English
Publishing date	2020-01-16
Publishing country	England
Document type	Journal Article
ZDB-ID	1472881-3
ISSN	1364-548X ; 1359-7345 ; 0009-241X
ISSN (online)	1364-548X
ISSN	1359-7345 ; 0009-241X
DOI	10.1039/c9cc09554c
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Article: Purely inorganic frameworks based on polyoxometalate clusters with abundant phosphate groups: single-crystal to single-crystal structural transformation and remarkable proton conduction

Zhang, Shan / Lu, Ying / Sun, Xiu-Wei / Li, Zhuo / Dang, Tian-Yi / Zhang, Zhong / Tian, Hong-Rui / Liu, Shu-Xia

Chemical communications. 2020 Jan. 2, v. 56, no. 3

2020

Abstract: A pure-inorganic framework based on {P₄Moⱽ₄Moⱽᴵ₂} clusters with rich phosphate groups has been synthesized. It underwent a single crystal to single crystal conversion in air to form a new framework with changes both in the metal valent state and ... ...

Abstract	A pure-inorganic framework based on {P₄Moⱽ₄Moⱽᴵ₂} clusters with rich phosphate groups has been synthesized. It underwent a single crystal to single crystal conversion in air to form a new framework with changes both in the metal valent state and coordination environment. The new framework exhibits an ultra-high proton conductivity of 1.33 × 10⁻² S cm⁻¹ at 95 °C and 98% relative humidity and excellent stability.
Keywords	air ; chemical reactions ; phosphates ; relative humidity
Language	English
Dates of publication	2020-0102
Size	p. 391-394.
Publishing place	The Royal Society of Chemistry
Document type	Article
ZDB-ID	1472881-3
ISSN	1364-548X ; 1359-7345 ; 0009-241X
ISSN (online)	1364-548X
ISSN	1359-7345 ; 0009-241X
DOI	10.1039/c9cc08696j
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Article ; Online: A multicentre synergistic polyoxometalate-based metal–organic framework for one-step selective oxidative cleavage of β-O-4 lignin model compounds

Tian, Hong-Rui / Liu, Yi-Wei / Zhang, Zhong / Liu, Shumei / Dang, Tian-Yi / Li, Xiao-Hui / Sun, Xiu-Wei / Lü, Ying / Liu, Shu-Xia

Green chemistry. 2020 Jan. 2, v. 22, no. 1 p.248-255

2020

Abstract: A novel mixed-valence polyoxovanadate-based copper–organic framework, [Cuᴵ(bbi)]₂{[Cuᴵ(bbi)]₂VIV2Vⱽ₈O₂₆}·2H₂O (NENU-MV-5, bbi = 1,1′-(1,4-butanediyl)bis(imidazole)), was facilely synthesized from routine reagents under mild hydrothermal conditions. Using ...

Abstract	A novel mixed-valence polyoxovanadate-based copper–organic framework, [Cuᴵ(bbi)]₂{[Cuᴵ(bbi)]₂VIV2Vⱽ₈O₂₆}·2H₂O (NENU-MV-5, bbi = 1,1′-(1,4-butanediyl)bis(imidazole)), was facilely synthesized from routine reagents under mild hydrothermal conditions. Using NENU-MV-5 as a heterogeneous catalyst without any co-catalyst, one-step oxidative cleavage of β-O-4 lignin into phenols and aromatic acids with high catalytic activity and selectivity was realized under an oxygen atmosphere. No obvious decrease in activity was observed after five cycles, which indicates the excellent stability and sustainability of NENU-MV-5. The perfect catalytic performance of NENU-MV-5 can be attributed to the multi-site synergistic effect of the mixed-valence Vⱽ–O–Vᴵⱽ sites on polyoxovanadate for the oxidation of β-O-4 alcohol to β-O-4 ketone and the Cu(i) sites on the framework for the rapid cleavage of the Cα–Cᵦ bond of β-O-4 ketone. This system represented the first co-catalyst-free example for the one-step selective degradation of lignin catalyzed by a well-defined crystalline catalyst with definite composition and structure in a single solvent.
Keywords	aromatic acids ; catalysts ; catalytic activity ; coordination polymers ; copper ; green chemistry ; imidazole ; lignin ; models ; oxidation ; oxygen ; phenols ; solvents ; synergism
Language	English
Dates of publication	2020-0102
Size	p. 248-255.
Publishing place	The Royal Society of Chemistry
Document type	Article ; Online
ZDB-ID	2006274-6
ISSN	1463-9270 ; 1463-9262
ISSN (online)	1463-9270
ISSN	1463-9262
DOI	10.1039/c9gc03626a
Database	NAL-Catalogue (AGRICOLA)

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