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Author |
Yang, S.; Liu, Z.; An, H.; Arnouts, S.; de Ruiter, J.; Rollier, F.; Bals, S.; Altantzis, T.; Figueiredo, M.C.; Filot, I.A.W.; Hensen, E.J.M.; Weckhuysen, B.M.; van der Stam, W. |
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Title |
Near-unity electrochemical CO₂ to CO conversion over Sn-doped copper oxide nanoparticles |
Type |
A1 Journal article |
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Year  |
2022 |
Publication |
ACS catalysis |
Abbreviated Journal |
Acs Catal |
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Volume |
12 |
Issue |
24 |
Pages |
15146-15156 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
Bimetallic electrocatalysts have emerged as a viable strategy to tune the electrocatalytic CO2 reduction reaction (eCO2RR) for the selective production of valuable base chemicals and fuels. However, obtaining high product selectivity and catalyst stability remain challenging, which hinders the practical application of eCO2RR. In this work, it was found that a small doping concentration of tin (Sn) in copper oxide (CuO) has profound influence on the catalytic performance, boosting the Faradaic efficiency (FE) up to 98% for carbon monoxide (CO) at -0.75 V versus RHE, with prolonged stable performance (FE > 90%) for up to 15 h. Through a combination of ex situ and in situ characterization techniques, the in situ activation and reaction mechanism of the electrocatalyst at work was elucidated. In situ Raman spectroscopy measurements revealed that the binding energy of the crucial adsorbed *CO intermediate was lowered through Sn doping, thereby favoring gaseous CO desorption. This observation was confirmed by density functional theory, which further indicated that hydrogen adsorption and subsequent hydrogen evolution were hampered on the Sn-doped electrocatalysts, resulting in boosted CO formation. It was found that the pristine electrocatalysts consisted of CuO nanoparticles decorated with SnO2 domains, as characterized by ex situ high-resolution scanning transmission electron microscopy and X-ray photoelectron spectroscopy measurements. These pristine nanoparticles were subsequently in situ converted into a catalytically active bimetallic Sn-doped Cu phase. Our work sheds light on the intimate relationship between the bimetallic structure and catalytic behavior, resulting in stable and selective oxide-derived Sn-doped Cu electrocatalysts. |
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Wos |
000900052400001 |
Publication Date |
2022-11-28 |
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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 |
2155-5435 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.9 |
Times cited |
16 |
Open Access |
OpenAccess |
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Notes |
B.M.W., S.Y., M.C.F., E.J.M.H., and W.v.d.S. acknowledge support from the Strategic UU-TU/e Alliance project ?Joint Centre for Chemergy Research?. S.B. acknowledges support from the European Research Council (ERC Consolidator grant #815128 REALNANO) . Z.L. acknowledges financial support of the China Scholarship Council and the Netherlands Organization for Scientific Research for access to computa-tional resources for carrying out the DFT calculations reported in this work. S.A. and T.A. acknowledge funding from theUniversity of Antwerp Research fund (BOF) . The authors also thank Dr. Jochem Wijten and Joris Janssens (Inorganic Chemistry and Catalysis, Utrecht University) for helpful technical support. Sander Deelen (Faculty of Science, Utrecht University) is acknowledged for the design of the in situ XRD cell. |
Approved |
Most recent IF: 12.9 |
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Call Number |
UA @ admin @ c:irua:192742 |
Serial |
7325 |
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Author |
Chaves, A.; Azadani, J.G.; Alsalman, H.; da Costa, D.R.; Frisenda, R.; Chaves, A.J.; Song, S.H.; Kim, Y.D.; He, D.; Zhou, J.; Castellanos-Gomez, A.; Peeters, F.M.; Liu, Z.; Hinkle, C.L.; Oh, S.-H.; Ye, P.D.; Koester, S.J.; Lee, Y.H.; Avouris, P.; Wang, X.; Low, T. |
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Title |
Bandgap engineering of two-dimensional semiconductor materials |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
npj 2D Materials and Applications |
Abbreviated Journal |
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Volume |
4 |
Issue |
1 |
Pages |
29-21 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
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Abstract |
Semiconductors are the basis of many vital technologies such as electronics, computing, communications, optoelectronics, and sensing. Modern semiconductor technology can trace its origins to the invention of the point contact transistor in 1947. This demonstration paved the way for the development of discrete and integrated semiconductor devices and circuits that has helped to build a modern society where semiconductors are ubiquitous components of everyday life. A key property that determines the semiconductor electrical and optical properties is the bandgap. Beyond graphene, recently discovered two-dimensional (2D) materials possess semiconducting bandgaps ranging from the terahertz and mid-infrared in bilayer graphene and black phosphorus, visible in transition metal dichalcogenides, to the ultraviolet in hexagonal boron nitride. In particular, these 2D materials were demonstrated to exhibit highly tunable bandgaps, achieved via the control of layers number, heterostructuring, strain engineering, chemical doping, alloying, intercalation, substrate engineering, as well as an external electric field. We provide a review of the basic physical principles of these various techniques on the engineering of quasi-particle and optical bandgaps, their bandgap tunability, potentials and limitations in practical realization in future 2D device technologies. |
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Wos |
000565588500001 |
Publication Date |
2020-08-24 |
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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 |
2397-7132 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
329 |
Open Access |
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Notes |
; Discussions and interactions with D.R. Reichman, F. Tavazza, N.M.R. Peres, and K. Choudhary are gratefully acknowledged. A.C. acknowledges financial support by CNPq, through the PRONEX/FUNCAP and PQ programs. This project has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (grant agreement No. 755655, ERCStG 2017 project 2D-TOPSENSE). Computational support from the Minnesota Supercomputing Institute (MSI) and EU Graphene Flagship funding (Grant Graphene Core 2, 785219) is acknowledged. R.F. acknowledges support from the Netherlands Organization for Scientific Research (NWO) through the research program Rubicon with project number 680-50-1515. D.H., J.Z., and X.W. acknowledge support by National Natural Science Foundation of China 61734003, 61521001, 61704073, 51861145202, and 61851401, and National Key Basic Research Program of China 2015CB921600 and 2018YFB2200500. J.Z. and Z.L. acknowledge support by RG7/18, MOE2017-T2-2-136, MOE2018-T3-1-002, and A*Star QTE program. S.H.S. and Y.H.L. acknowledge the support from IBS-R011-D1. Y.D.K. is supported by Samsung Research and Incubation Funding Center of Samsung Electronics under Project Number SRFC-TB1803-04. S.J.K acknowledges financial support by the National Science Foundation (NSF), under award DMR-1921629. T.L. and J.G.A. acknowledge funding support from NSF/DMREF under Grant Agreement No. 1921629. S.-H.O. acknowledges support from the U.S. National Science Foundation (NSF ECCS 1809723) and Samsung Global Research Outreach (GRO) project. ; |
Approved |
Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:172069 |
Serial |
6459 |
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Author |
Liu, F.; Meng, J.; Xia, F.; Liu, Z.; Peng, H.; Sun, C.; Xu, L.; Van Tendeloo, G.; Mai, L.; Wu, J. |
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Title |
Origin of the extra capacity in nitrogen-doped porous carbon nanofibers for high-performance potassium ion batteries |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Journal Of Materials Chemistry A |
Abbreviated Journal |
J Mater Chem A |
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Volume |
8 |
Issue |
35 |
Pages |
18079-18086 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
While graphite has limited capacity as an anode material for potassium-ion batteries, nitrogen-doped carbon materials are more promising as extra capacity can usually be produced. However, the mechanism behind the origin of the extra capacity remains largely unclear. Here, the potassium storage mechanisms have been systematically studied in freestanding and porous N-doped carbon nanofibers with an additional similar to 100 mA h g(-1)discharge capacity at 0.1 A g(-1). The extra capacity is generated in the whole voltage window range from 0.01 to 2 V, which corresponds to both surface/interface K-ion absorptions due to the pyridinic N and pyrrolic N induced atomic vacancies and layer-by-layer intercalation due to the effects of graphitic N. As revealed by transmission electron microscopy, the N-doped samples have a clear and enhanced K-intercalation reaction. Theoretical calculations confirmed that the micropores with pyridinic N and pyrrolic N provide extra sites to form bonds with K, resulting in the extra capacity at high voltage. The chemical absorption of K-ions occurring inside the defective graphitic layer will prompt fast diffusion of K-ions and full realization of the intercalation capacity at low voltage. The approach of preparing N-doped carbon-based materials and the mechanism revealed by this work provide directions for the development of advanced materials for efficient energy storage. |
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Corporate Author |
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Wos |
000569873400015 |
Publication Date |
2020-08-03 |
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Abbreviated Series Title |
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Series Issue |
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Edition |
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ISSN |
2050-7488; 2050-7496 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
11.9 |
Times cited |
2 |
Open Access |
OpenAccess |
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Notes |
; F. Liu and J. S. Meng contributed equally to this work. This work was supported by the National Natural Science Foundation of China (51832004 and 51521001), the National Key Research and Development Program of China (2016YFA0202603), and the Natural Science Foundation of Hubei Province (2019CFA001). The S/TEM work was performed at the Nanostructure Research Center (NRC), which is supported by the Fundamental Research Funds for the Central Universities (WUT: 2019III012GX, 2020III002GX), the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, and the State Key Laboratory of Silicate Materials for Architectures (all of the laboratories are at Wuhan University of Technology). ; |
Approved |
Most recent IF: 11.9; 2020 IF: 8.867 |
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Call Number |
UA @ admin @ c:irua:172741 |
Serial |
6573 |
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Author |
Yang, X.-Y.; Tian, G.; Chen, L.-H.; Li, Y.; Rooke, J.C.; Wei, Y.-X.; Liu, Z.-M.; Deng, Z.; Van Tendeloo, G.; Su, B.-L. |
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Title |
Well-organized zeolite nanocrystal aggregates with interconnected hierarchically micro-meso-macropore systems showing enhanced catalytic performance |
Type |
A1 Journal article |
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Year |
2011 |
Publication |
Chemistry: a European journal |
Abbreviated Journal |
Chem-Eur J |
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Volume |
17 |
Issue |
52 |
Pages |
14987-14995 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Preparation and characterization of well-organized zeolitic nanocrystal aggregates with an interconnected hierarchically micromesomacro porous system are described. Amorphous nanoparticles in bimodal aluminosilicates were directly transformed into highly crystalline nanosized zeolites, as well as acting as scaffold template. All pores on three length scales incorporated in one solid body are interconnected with each other. These zeolitic nanocrystal aggregates with hierarchically micromesomacroporous structure were thoroughly characterized. TEM images and 29Si NMR spectra showed that the amorphous phase of the initial material had been completely replaced by nanocrystals to give a micromesomacroporous crystalline zeolitic structure. Catalytic testing demonstrated their superiority due to the highly active sites and the presence of interconnected micromesomacroporosity in the cracking of bulky 1,3,5-triisopropylbenzene (TIPB) compared to traditional zeolite catalysts. This synthesis strategy was extended to prepare various zeolitic nanocrystal aggregates (ZSM-5, Beta, TS-1, etc.) with well-organized hierarchical micromesomacroporous structures. |
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Place of Publication |
Weinheim |
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Wos |
000298547300035 |
Publication Date |
2011-11-23 |
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Abbreviated Series Title |
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Series Issue |
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Edition |
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ISSN |
0947-6539; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
5.317 |
Times cited |
61 |
Open Access |
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Notes |
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Approved |
Most recent IF: 5.317; 2011 IF: 5.925 |
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Call Number |
UA @ lucian @ c:irua:96274 |
Serial |
3913 |
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Author |
Laffez, P.; Chen, X.Y.; Banerjee, G.; Pezeril, T.; Rossell, M.D.; Van Tendeloo, G.; Lacorre, P.; Liu, J.M.; Liu, Z.-G. |
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Title |
Growth of La2Mo2O9 films on porous Al2O3 substrates by radio frequency magnetron sputtering |
Type |
A1 Journal article |
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Year |
2006 |
Publication |
Thin solid films : an international journal on the science and technology of thin and thick films |
Abbreviated Journal |
Thin Solid Films |
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Volume |
500 |
Issue |
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Pages |
27-33 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Place of Publication |
Lausanne |
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Wos |
000235764600006 |
Publication Date |
2005-12-16 |
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Abbreviated Series Title |
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Edition |
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ISSN |
0040-6090; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
1.879 |
Times cited |
15 |
Open Access |
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Notes |
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Approved |
Most recent IF: 1.879; 2006 IF: 1.666 |
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Call Number |
UA @ lucian @ c:irua:57000 |
Serial |
1396 |
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Author |
Cao, L.-H.; Yu, W.; Xu, H.; Zheng, C.-Y.; Liu, Z.-J.; Li, B.; Bogaerts, A. |
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Title |
Terahertz radiation from oscillating electrons in laser-induced wake fields |
Type |
A1 Journal article |
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Year |
2004 |
Publication |
Physical review : E : statistical physics, plasmas, fluids, and related interdisciplinary topics |
Abbreviated Journal |
Phys Rev E |
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Volume |
70 |
Issue |
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Pages |
046408,1-7 |
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Keywords |
A1 Journal article; Condensed Matter Theory (CMT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Strong terahertz (1THz=1012Hz) radiation can be generated by the electron oscillation in fs-laser-induced wake fields. The interaction of a fs-laser pulse with a low-density plasma layer is studied in detail using numerical simulations. The spatial distribution and temporal evolution of terahertz electron current developed in a low-density plasma layer are presented, which enables us to calculate the intensity distribution of THz radiation. It is shown that laser and plasma parameters, such as laser intensity, pulse width, and background plasma density, are of key importance to the process. The optimum condition for wake-field excitation and terahertz emission is discussed upon the simulation results. Radiation peaked at 6.4 THz, with 900 fs duration and 9% bandwidth, can be generated in a plasma of density 5×1017cm−3. It turns out that the maximum radiation intensity scales as n03a04 when wake field is resonantly excited, where n0 and a0 are, respectively, the plasma density and the normalized field amplitude of the laser pulse. |
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Place of Publication |
Lancaster, Pa |
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Wos |
000225689600086 |
Publication Date |
2004-10-14 |
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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 |
1539-3755;1550-2376; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
2.366 |
Times cited |
9 |
Open Access |
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Notes |
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Approved |
Most recent IF: 2.366; 2004 IF: NA |
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Call Number |
UA @ lucian @ c:irua:49818 |
Serial |
3509 |
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