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Records |
Links |
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Author |
Ying, J.; Xiao, Y.; Chen, J.; Hu, Z.-Y.; Tian, G.; Van Tendeloo, G.; Zhang, Y.; Symes, M.D.D.; Janiak, C.; Yang, X.-Y. |
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Title |
Fractal design of hierarchical PtPd with enhanced exposed surface atoms for highly catalytic activity and stability |
Type |
A1 Journal article |
| |
Year  |
2023 |
Publication |
Nano letters |
Abbreviated Journal |
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| |
Volume |
23 |
Issue |
16 |
Pages |
7371-7378 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Hierarchicalassembly of arc-like fractal nanostructures not onlyhas its unique self-similarity feature for stability enhancement butalso possesses the structural advantages of highly exposed surface-activesites for activity enhancement, remaining a great challenge for high-performancemetallic nanocatalyst design. Herein, we report a facile strategyto synthesize a novel arc-like hierarchical fractal structure of PtPdbimetallic nanoparticles (h-PtPd) by using pyridinium-type ionic liquidsas the structure-directing agent. Growth mechanisms of the arc-likenanostructured PtPd nanoparticles have been fully studied, and precisecontrol of the particle sizes and pore sizes has been achieved. Dueto the structural features, such as size control by self-similaritygrowth of subunits, structural stability by nanofusion of subunits,and increased numbers of exposed active atoms by the curved homoepitaxialgrowth, h-PtPd displays outstanding electrocatalytic activity towardoxygen reduction reaction and excellent stability during hydrothermaltreatment and catalytic process. |
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Corporate Author |
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Thesis |
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Place of Publication |
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Editor |
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Wos |
001042181100001 |
Publication Date |
2023-08-03 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
1530-6984 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
10.8 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
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Approved |
Most recent IF: 10.8; 2023 IF: 12.712 |
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| |
Call Number |
UA @ admin @ c:irua:198408 |
Serial |
8870 |
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| Permanent link to this record |
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Author |
Liu, J.-W.; Wu, S.-M.; Wang, L.-Y.; Tian, G.; Qin, Y.; Wu, J.-X.; Zhao, X.-F.; Zhang, Y.-X.; Chang, G.-G.; Wu, L.; Zhang, Y.-X.; Li, Z.-F.; Guo, C.-Y.; Janiak, C.; Lenaerts, S.; Yang, X.-Y. |
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Title |
Pd/Lewis acid synergy in macroporous Pd@Na-ZSM-5 for enhancing selective conversion of biomass |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Chemcatchem |
Abbreviated Journal |
Chemcatchem |
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| |
Volume |
|
Issue |
|
Pages |
1-6 |
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| |
Keywords |
A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
Pd nanometal particles encapsulated in macroporous Na-ZSM-5 with only Lewis acid sites have been successfully synthesized by a steam-thermal approach. The synergistic effect of Pd and Lewis acid sites have been investigated for significant enhancement of the catalytic selectivity towards furfural alcohol in furfural hydroconversion. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000554645800001 |
Publication Date |
2020-07-11 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
1867-3880; 1867-3899 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
4.5 |
Times cited |
1 |
Open Access |
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Notes |
; We acknowledge a joint DFG-NSFC project (DFG JA466/39-1, NSFC grant 51861135313). This work was also supported by National Key R&D Program of China (2017YFC1103800), NSFC (U1662134, 21711530705), Jilin Province Science and Technology Development Plan (20180101208JC), HPNSF (2016CFA033), FRFCU (19lgzd16) and ISTCP (2015DFE52870). ; |
Approved |
Most recent IF: 4.5; 2020 IF: 4.803 |
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| |
Call Number |
UA @ admin @ c:irua:171178 |
Serial |
6579 |
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| Permanent link to this record |
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Author |
Lu, Y.; Liu, X.-L.; He, L.; Zhang, Y.-X.; Hu, Z.-Y.; Tian, G.; Cheng, X.; Wu, S.-M.; Li, Y.-Z.; Yang, X.-H.; Wang, L.-Y.; Liu, J.-W.; Janiak, C.; Chang, G.-G.; Li, W.-H.; Van Tendeloo, G.; Yang, X.-Y.; Su, B.-L. |
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Title |
Spatial heterojunction in nanostructured TiO₂ and its cascade effect for efficient photocatalysis |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Nano Letters |
Abbreviated Journal |
Nano Lett |
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| |
Volume |
20 |
Issue |
5 |
Pages |
3122-3129 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
A highly efficient photoenergy conversion is strongly dependent on the cumulative cascade efficiency of the photogenerated carriers. Spatial heterojunctions are critical to directed charge transfer and, thus, attractive but still a challenge. Here, a spatially ternary titanium-defected TiO2@carbon quantum dots@reduced graphene oxide (denoted as V-Ti@CQDs@rGO) in one system is shown to demonstrate a cascade effect of charges and significant performances regarding the photocurrent, the apparent quantum yield, and photocatalysis such as H-2 production from water splitting and CO2 reduction. A key aspect in the construction is the technologically irrational junction of Ti-vacancies and nanocarbons for the spatially inside-out heterojunction. The new “spatial heterojunctions” concept, characteristics, mechanism, and extension are proposed at an atomic- nanoscale to clarify the generation of rational heterojunctions as well as the cascade electron transfer. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000535255300024 |
Publication Date |
2020-04-28 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
1530-6984 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
10.8 |
Times cited |
5 |
Open Access |
Not_Open_Access |
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| |
Notes |
; This work was supported by the joint National Natural Science Foundation of China-Deutsche Forschungsgemeinschaft (NSFC-DFG) project (NSFC grant 51861135313, DFG JA466/39-1), Fundamental Research Funds for the Central Universities (19lgpy113, 19lgzd16), Program for Changjiang Scholars and Innovative Research Team in University (IRT_15R52) and Jilin Province Science and Technology Development Plan (20180101208JC). ; |
Approved |
Most recent IF: 10.8; 2020 IF: 12.712 |
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| |
Call Number |
UA @ admin @ c:irua:170263 |
Serial |
6608 |
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| Permanent link to this record |
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Author |
Lu, Y.; Liu, Y.-X.; He, L.; Wang, L.-Y.; Liu, X.-L.; Liu, J.-W.; Li, Y.-Z.; Tian, G.; Zhao, H.; Yang, X.-H.; Liu, J.; Janiak, C.; Lenaerts, S.; Yang, X.-Y.; Su, B.-L. |
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Title |
Interfacial co-existence of oxygen and titanium vacancies in nanostructured TiO₂ for enhancement of carrier transport |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Nanoscale |
Abbreviated Journal |
Nanoscale |
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| |
Volume |
12 |
Issue |
15 |
Pages |
8364-8370 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) |
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| |
Abstract |
The interfacial co-existence of oxygen and metal vacancies in metal oxide semiconductors and their highly efficient carrier transport have rarely been reported. This work reports on the co-existence of oxygen and titanium vacancies at the interface between TiO2 and rGO via a simple two-step calcination treatment. Experimental measurements show that the oxygen and titanium vacancies are formed under 550 degrees C/Ar and 350 degrees C/air calcination conditions, respectively. These oxygen and titanium vacancies significantly enhance the transport of interfacial carriers, and thus greatly improve the photocurrent performances, the apparent quantum yield, and photocatalysis such as photocatalytic H-2 production from water-splitting, photocatalytic CO2 reduction and photo-electrochemical anticorrosion of metals. A new “interfacial co-existence of oxygen and titanium vacancies” phenomenon, and its characteristics and mechanism are proposed at the atomic-/nanoscale to clarify the generation of oxygen and titanium vacancies as well as the interfacial carrier transport. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000529201500029 |
Publication Date |
2020-02-26 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
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| |
ISSN |
2040-3364 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
6.7 |
Times cited |
4 |
Open Access |
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| |
Notes |
; This work was supported by the National Natural Science Foundation of China (51861135313, U1663225, U1662134, and 51472190), the International Science & Technology Cooperation Program of China (2015DFE52870), the Program for Changjiang Scholars and Innovative Research Team in University (IRT_15R52), the Fundamental Research Funds for the Central Universities (19lgpy113 and 19lgzd16), the Jilin Province Science and Technology Development Plan (20180101208JC) and the Hubei Provincial Natural Science Foundation of China (2016CFA033). ; |
Approved |
Most recent IF: 6.7; 2020 IF: 7.367 |
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| |
Call Number |
UA @ admin @ c:irua:169578 |
Serial |
6550 |
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| Permanent link to this record |
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Author |
Wu, S.-M.; Liu, X.-L.; Lian, X.-L.; Tian, G.; Janiak, C.; Zhang, Y.-X.; Lu, Y.; Yu, H.-Z.; Hu, J.; Wei, H.; Zhao, H.; Chang, G.-G.; Van Tendeloo, G.; Wang, L.-Y.; Yang, X.-Y.; Su, B.-L. |
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Title |
Homojunction of oxygen and titanium vacancies and its interfacial n-p effect |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Advanced materials |
Abbreviated Journal |
Adv Mater |
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| |
Volume |
30 |
Issue |
32 |
Pages |
1802173 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
The homojunction of oxygen/metal vacancies and its interfacial n-p effect on the physiochemical properties are rarely reported. Interfacial n-p homojunctions of TiO2 are fabricated by directly decorating interfacial p-type titanium-defected TiO2 around n-type oxygen-defected TiO2 nanocrystals in amorphous-anatase homogeneous nanostructures. Experimental measurements and theoretical calculations on the cell lattice parameters show that the homojunction of oxygen and titanium vacancies changes the charge density of TiO2; a strong EPR signal caused by oxygen vacancies and an unreported strong titanium vacancies signal of 2D H-1 TQ-SQ MAS NMR are present. Amorphous-anatase TiO2 shows significant performance regarding the photogeneration current, photocatalysis, and energy storage, owing to interfacial n-type to p-type conductivity with high charge mobility and less structural confinement of amorphous clusters. A new homojunction of oxygen and titanium vacancies concept, characteristics, and mechanism are proposed at an atomic-/nanoscale to clarify the generation of oxygen vacancies and titanium vacancies as well as the interface electron transfer. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Weinheim |
Editor |
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Language |
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Wos |
000440813300022 |
Publication Date |
2018-06-27 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
0935-9648 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
19.791 |
Times cited |
39 |
Open Access |
Not_Open_Access |
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| |
Notes |
; This work was supported by National Key R&D Program of China (2017YFC1103800), National SFC (U1662134, U1663225, 51472190, 51611530672, 21711530705, 51503166, 21706199), ISTCP (2015DFE52870), PCSIRT (IRT_15R52), HPNSF (2016CFA033, 2017CFB487), and SKLPPC (PPC2016007). ; |
Approved |
Most recent IF: 19.791 |
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| |
Call Number |
UA @ lucian @ c:irua:153106 |
Serial |
5105 |
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| Permanent link to this record |
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Author |
Xiao, S.; Lu, Y.; Xiao, B.-Y.; Wu, L.; Song, J.-P.; Xiao, Y.-X.; Wu, S.-M.; Hu, J.; Wang, Y.; Chang, G.-G.; Tian, G.; Lenaerts, S.; Janiak, C.; Yang, X.-Y.; Su, B.-L. |
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Title |
Hierarchically dual-mesoporous TiO2 microspheres for enhanced photocatalytic properties and lithium storage |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Chemistry: a European journal |
Abbreviated Journal |
Chem-Eur J |
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| |
Volume |
24 |
Issue |
50 |
Pages |
13246-13252 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
Hierarchically dual‐mesoporous TiO2 microspheres have been synthesized via a solvothermal process in the presence of 1‐butyl‐3‐methylmidazolium tetrafluoroborate ([BMIm][BF4]) and diethylenetriamine (DETA) as co‐templates. Secondary mesostructured defects in the hierarchical TiO2 microspheres produce the oxygen vacancies, which not only significantly enhance the photocatalytic activity on degrading methyl blue (over 1.7 times to P25) and acetone (over 2.9 times of P25), but which also are beneficial for lithium storage. Moreover, we propose a mechanism to obtain a better understanding of the role of dual mesoporosity of TiO2 microspheres for enhancing the molecular diffusion, ion transportation and electron transformation. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000443804100025 |
Publication Date |
2018-06-21 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
0947-6539 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
5.317 |
Times cited |
6 |
Open Access |
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Notes |
; This work is supported by the National Key R&D Program of China (2017YFC1103800), the Program for Changjiang Scholars and Innovative Research Team in University (IRT 15R52), the National Natural Science Foundation of China (U1662134, U1663225, 51472190, 51611530672, 51503166, 21706199, 21711530705), the International Science & Technology Cooperation Program of China (2015DFE52870), the Natural Science Foundation of Hubei Province (2016CFA033, 2017CFB487), the Open Project Program of State Key Laboratory of Petroleum Pollution Control (PPC2016007), and the CNPC Research Institute of Safety and Environmental Technology. ; |
Approved |
Most recent IF: 5.317 |
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| |
Call Number |
UA @ admin @ c:irua:151812 |
Serial |
5957 |
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| Permanent link to this record |
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Author |
Dong, Y.; Chen, S.-Y.; Lu, Y.; Xiao, Y.-X.; Hu, J.; Wu, S.-M.; Deng, Z.; Tian, G.; Chang, G.-G.; Li, J.; Lenaerts, S.; Janiak, C.; Yang, X.-Y.; Su, B.-L. |
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Title |
Hierarchical MoS2@TiO2 heterojunctions for enhanced photocatalytic performance and electrocatalytic hydrogen evolution |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Chemistry: an Asian journal |
Abbreviated Journal |
Chem-Asian J |
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| |
Volume |
13 |
Issue |
12 |
Pages |
1609-1615 |
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Keywords |
A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
Hierarchical MoS2@TiO2 heterojunctions were synthesized through a one-step hydrothermal method by using protonic titanate nanosheets as the precursor. The TiO2 nanosheets prevent the aggregation of MoS2 and promote the carrier transfer efficiency, and thus enhance the photocatalytic and electrocatalytic activity of the nanostructured MoS2. The obtained MoS2@TiO2 has significantly enhanced photocatalytic activity in the degradation of rhodamineB (over 5.2times compared with pure MoS2) and acetone (over 2.8times compared with pure MoS2). MoS2@TiO2 is also beneficial for electrocatalytic hydrogen evolution (26times compared with pure MoS2, based on the cathodic current density). This work offers a promising way to prevent the self-aggregation of MoS2 and provides a new insight for the design of heterojunctions for materials with lattice mismatches. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000435773300011 |
Publication Date |
2018-04-10 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
1861-4728; 1861-471x |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
4.083 |
Times cited |
22 |
Open Access |
|
|
| |
Notes |
; This work was supported by the National Key R&D Program of China (2017YFC1103800), PCSIRT (IRT15R52), NSFC (U1662134, U1663225, 51472190, 51611530672, 51503166, 21706199, 21711530705), ISTCP (2015DFE52870), HPNSF (2016CFA033, 2017CFB487), and SKLPPC (PPC2016007). ; |
Approved |
Most recent IF: 4.083 |
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| |
Call Number |
UA @ admin @ c:irua:151971 |
Serial |
5956 |
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| Permanent link to this record |
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Author |
Wei, H.; Hu, Z.-Y.; Xiao, Y.-X.; Tian, G.; Ying, J.; Van Tendeloo, G.; Janiak, C.; Yang, X.-Y.; Su, B.-L. |
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Title |
Control of the interfacial wettability to synthesize highly dispersed PtPd nanocrystals for efficient oxygen reduction reaction |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Chemistry: an Asian journal |
Abbreviated Journal |
Chem-Asian J |
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Volume |
13 |
Issue |
9 |
Pages |
1119-1123 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Highly dispersed PtPd bimetallic nanocrystals with enhanced catalytic activity and stability were prepared by adjusting the interfacial wettability of the reaction solution on a commercial carbon support. This approach holds great promise for the development of high-performance and low-cost catalysts for practical applications. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Weinheim |
Editor |
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| |
Language |
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Wos |
000431625200006 |
Publication Date |
2018-03-24 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
1861-4728; 1861-471x |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
4.083 |
Times cited |
3 |
Open Access |
Not_Open_Access |
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| |
Notes |
; This work supported by National Key R&D Program of China (2017YFC1103800), PCSIRT (IRT15R52), NSFC (U1663225, U1662134, 51472190, 51611530672, 21711530705, 51503166), ISTCP (2015DFE52870), HPNSF (2016CFA033, 2017CFB487), and Open Project Program of State Key Laboratory of Petroleum Pollution Control (Grant No. PPC2016007), CNPC Research Institute of Safety and Environmental Technology, SKLPPC. ; |
Approved |
Most recent IF: 4.083 |
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| |
Call Number |
UA @ lucian @ c:irua:151525 |
Serial |
5018 |
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| Permanent link to this record |
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Author |
Ying, J.; Hu, Z.-Y.; Yang, X.-Y.; Wei, H.; Xiao, Y.-X.; Janiak, C.; Mu, S.-C.; Tian, G.; Pan, M.; Van Tendeloo, G.; Su, B.-L. |
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Title |
High viscosity to highly dispersed PtPd bimetallic nanocrystals for enhanced catalytic activity and stability |
Type |
A1 Journal article |
| |
Year |
2016 |
Publication |
Chemical communications |
Abbreviated Journal |
Chem Commun |
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| |
Volume |
52 |
Issue |
52 |
Pages |
8219-8222 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
A facile high-viscosity-solvent method is presented to synthesize PtPd bimetallic nanocrystals highly dispersed in different mesostructures (2D and 3D structures), porosities (large and small pore sizes), and compositions (silica and carbon). Further, highly catalytic activity, stability and durability of the nanometals have been proven in different catalytic reactions. |
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Address |
State Key Laboratory Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, 122, Luoshi Road, Wuhan, 430070, China. xyyang@whut.edu.cn |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
English |
Wos |
000378715400006 |
Publication Date |
2016-05-16 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
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| |
ISSN |
1359-7345 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
6.319 |
Times cited |
19 |
Open Access |
|
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| |
Notes |
This work was supported by NFSC (51472190 and 51503166), ISTCP (2015DFE52870), PCSIRT (IRT15R52) of China, and the Integrated Infrastructure Initiative of EU (312483-ESTEEM2).; esteem2jra4 |
Approved |
Most recent IF: 6.319 |
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| |
Call Number |
c:irua:134660 c:irua:134660 |
Serial |
4110 |
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| Permanent link to this record |
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Author |
Ying, J.; Yang, X.-Y.; Hu, Z.-Y.; Mu, S.-C.; Janiak, C.; Geng, W.; Pan, M.; Ke, X.; Van Tendeloo, G.; Su, B.-L. |
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Title |
One particle@one cell : highly monodispersed PtPd bimetallic nanoparticles for enhanced oxygen reduction reaction |
Type |
A1 Journal article |
| |
Year |
2014 |
Publication |
Nano energy |
Abbreviated Journal |
Nano Energy |
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| |
Volume |
8 |
Issue |
|
Pages |
214-222 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Highly monodispersed platinum-based nanoalloys are the best-known catalysts for the oxygen reduction reaction. Although certainly promising, the durability and stability are among the main requirements for commercializing fuel cell electrocatalysts in practical applications. Herein, we synthesize highly stable, durable and catalytic active monodispersed PtPd nano-particles encapsulated in a unique one particle@one cell structure by adjusting the viscosity of solvents using mesocellular foam. PtPd nanoparticles in mesocellular carbon foam exhibit an excellent electrocatalytic activity (over 4 times mass and specific activities than the commercial Pt/C catalyst). Most importantly, this nanocatalyst shows no obvious change of structure and only a 29.5% loss in electrochemically active surface area after 5000 potential sweeps between 0.6 and 1.1 V versus reversible hydrogen electrode cycles. (C) 2014 Elsevier Ltd. All rights reserved. |
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Wos |
000340981700026 |
Publication Date |
2014-06-23 |
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2211-2855; |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.343 |
Times cited |
40 |
Open Access |
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Approved |
Most recent IF: 12.343; 2014 IF: 10.325 |
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Call Number |
UA @ lucian @ c:irua:119255 |
Serial |
2465 |
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Author |
Schütte, K.; Doddi, A.; Kroll, C.; Meyer, H.; Wiktor, C.; Gemel, C.; Van Tendeloo, G.; Fischer, R.A.; Janiak, C. |
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Title |
Colloidal nickel/gallium nanoalloys obtained from organometallic precursors in conventional organic solvents and in ionic liquids : noble-metal-free alkyne semihydrogenation catalysts |
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A1 Journal article |
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Year |
2014 |
Publication |
Nanoscale |
Abbreviated Journal |
Nanoscale |
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Volume |
6 |
Issue |
10 |
Pages |
5532-5544 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Efforts to replace noble-metal catalysts by low-cost alternatives are of constant interest. The organometallic, non-aqueous wet-chemical synthesis of various hitherto unknown nanocrystalline Ni/Ga intermetallic materials and the use of NiGa for the selective semihydrogenation of alkynes to alkenes are reported. Thermal co-hydrogenolysis of the all-hydrocarbon precursors [Ni(COD)(2)] (COD = 1,5-cyclooctadiene) and GaCp* (Cp* = pentamethylcyclopentadienyl) in high-boiling organic solvents mesitylene and n-decane in molar ratios of 1 : 1, 2 : 3 and 3 : 1 yields the nano-crystalline powder materials of the over-all compositions NiGa, Ni2Ga3 and Ni3Ga, respectively. Microwave induced co-pyrolysis of the same precursors without additional hydrogen in the ionic liquid [BMIm][BF4] (BMIm = 1-butyl-3-methyl-imidazolium) selectively yields the intermetallic phases NiGa and Ni3Ga from the respective 1 : 1 and 3 : 1 molar ratios of the precursors. The obtained materials are characterized by transmission electron microscopy (TEM), energy dispersive X-ray spectroscopy (EDX), IR, powder X-ray diffraction (PXRD) and atomic absorption spectroscopy (AAS). The single-source precursor [Ni(GaCp*)(PMe3)(3)] with a fixed Ni : Ga stoichiometry of 1 : 1 was employed as well. In comparison with the co-hydrogenolytic dual precursor source approach it turned out to be less practical due to inefficient nickel incorporation caused by the parasitic formation of stable [Ni(PMe3)(4)]. The use of ionic liquid [BMIm][BF4] as a non-conventional solvent to control the reaction and stabilize the nanoparticles proved to be particularly advantageous and stable colloids of the nanoalloys NiGa and Ni3Ga were obtained. A phase-selective Ni/Ga colloid synthesis in conventional solvents and in the presence of surfactants such as hexadecylamine (HDA) was not feasible due to the undesired reactivity of HDA with GaCp* leading to inefficient gallium incorporation. Recyclable NiGa nanoparticles selectively semihydrogenate 1-octyne and diphenylacetylene (tolan) to 1-octene and diphenylethylene, respectively, with a yield of about 90% and selectivities of up to 94 and 87%. Ni-NPs yield alkanes with a selectivity of 97 or 78%, respectively, under the same conditions. |
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Cambridge |
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000335148800069 |
Publication Date |
2014-03-06 |
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ISSN |
2040-3364;2040-3372; |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.367 |
Times cited |
40 |
Open Access |
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Most recent IF: 7.367; 2014 IF: 7.394 |
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Call Number |
UA @ lucian @ c:irua:117251 |
Serial |
390 |
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