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Author |
Bigiani, L.; Barreca, D.; Gasparotto, A.; Andreu, T.; Verbeeck, J.; Sada, C.; Modin, E.; Lebedev, O.I.; Morante, J.R.; Maccato, C. |
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Title |
Selective anodes for seawater splitting via functionalization of manganese oxides by a plasma-assisted process |
Type |
A1 Journal article |
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Year  |
2021 |
Publication |
Applied Catalysis B-Environmental |
Abbreviated Journal |
Appl Catal B-Environ |
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Volume |
284 |
Issue |
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Pages |
119684 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The electrolysis of seawater, a significantly more abundant natural reservoir than freshwater, stands as a promising alternative for sustainable hydrogen production, provided that the competitive chloride electro-oxidation is minimized. Herein, we propose an original material combination to selectively trigger oxygen evolution from seawater at expenses of chlorine generation. The target systems, based on MnO2 or Mn2O3 decorated with Fe2O3 or Co3O4, are fabricated by plasma enhanced-chemical vapor deposition of manganese oxides, functionalization with Fe2O3 and Co3O4 by sputtering, and annealing in air/Ar to obtain Mn(IV)/Mn(III) oxides. Among the various options, MnO2 decorated with Co3O4 yields the best performances in alkaline seawater splitting, with an outstanding Tafel slope of approximate to 40 mV x dec(-1) and an overpotential of 450 mV, enabling to rule out chlorine evolution. These attractive performances, resulting from the synergistic contribution of catalytic and electronic effects, open the door to low-cost hydrogen generation from seawater under real-world conditions, paving the way to eventual large-scale applications. |
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Wos |
000623591500008 |
Publication Date |
2020-11-20 |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0926-3373 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.446 |
Times cited |
67 |
Open Access |
OpenAccess |
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Notes |
The authors thank Padova University (DOR 2017–2020 and P-DiSC #03BIRD2018-UNIPD OXYGENA projects), as well as the INSTM Consortium (INSTMPD004 – NETTUNO project) and AMGA Foundation (Mn4Energy project), for financial support. The Qu-Ant-EM microscope was partly funded by the Hercules fund from the Flemish Government. J.V. acknowledges funding from a GOA project 'Solarpaint' (University of Antwerp) and from the EU-H2020 programme (grant agreement No. 823717 – ESTEEM3). J.R.M. and T.A. acknowledge Generalitat de Catalunya for financial support through the CERCA Programme, 27 M2E (2017SGR1246) and by ERDEF-MINECO coordinated projects ENE2017-85087-C3 and ENE2016-80788-C5-5-R. Thanks are also due to Proff. Gloria Tabacchi and Ettore Fois (Department of Science and High Technology, Insubria University, Como, Italy) for valuable discussions and support. Dr. Daniele Valbusa, Dr. Gianluca Corrò, Dr. Andrea Gallo and Dr. Dileep Khrishnan are gratefully acknowledged for helpful technical assistance. |
Approved |
Most recent IF: 9.446 |
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Call Number |
UA @ admin @ c:irua:176718 |
Serial |
6733 |
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Author |
Bigiani, L.; Gasparotto, A.; Andreu, T.; Verbeeck, J.; Sada, C.; Modin, E.; Lebedev, O.I.; Morante, J.R.; Barreca, D.; Maccato, C. |
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Title |
Au-manganese oxide nanostructures by a plasma-assisted process as electrocatalysts for oxygen evolution : a chemico-physical investigation |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Advanced sustainable systems |
Abbreviated Journal |
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Volume |
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Issue |
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Pages |
2000177-11 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Earth-abundant and eco-friendly manganese oxides are promising platforms for the oxygen evolution reaction (OER) in water electrolysis. Herein, a versatile and potentially scalable route to gold-decorated manganese oxide-based OER electrocatalysts is reported. In particular, MnxOy(MnO2, Mn2O3) host matrices are grown on conductive glasses by plasma assisted-chemical vapor deposition (PA-CVD), and subsequently functionalized with gold nanoparticles (guest) as OER activators by radio frequency (RF)-sputtering. The final selective obtainment of MnO2- or Mn2O3-based systems is then enabled by annealing under oxidizing or inert atmosphere, respectively. A detailed material characterization evidences the formation of high-purity Mn(x)O(y)dendritic nanostructures with an open morphology and an efficient guest dispersion into the host matrices. The tailoring of Mn(x)O(y)phase composition and host-guest interactions has a remarkable influence on OER activity yielding, for the best performing Au/Mn(2)O(3)system, a current density of approximate to 5 mA cm(-2)at 1.65 V versus the reversible hydrogen electrode (RHE) and an overpotential close to 300 mV at 1 mA cm(-2). Such results, comparing favorably with literature data on manganese oxide-based materials, highlight the importance of compositional control, as well as of surface and interface engineering, to develop low-cost and efficient anode nanocatalysts for water splitting applications. |
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Wos |
000572376000001 |
Publication Date |
2020-09-25 |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2366-7486 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.1 |
Times cited |
4 |
Open Access |
Not_Open_Access |
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Notes |
; Padova University (DOR 2017-2019 and P-DiSC #03BIRD2018-UNIPD OXYGENA projects), as well as the INSTM Consortium (INSTMPD004 – NETTUNO project) and AMGA Foundation (Mn4Energy project), are gratefully acknowledged for financial support. The Qu-Ant-EM microscope was partially funded by the Hercules fund from the Flemish Government. J.V. acknowledges funding from a GOA project “Solarpaint” from the University of Antwerp and from EU H2020 823717 ESTEEM3 project. The authors thank Dr. Daniele Valbusa, Dr. Gianluca Corr, Dr. Andrea Gallo, and Dr. Dileep Khrishnan for helpful experimental assistance. ; esteem3TA; esteem3reported |
Approved |
Most recent IF: 7.1; 2020 IF: NA |
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Call Number |
UA @ admin @ c:irua:171937 |
Serial |
6457 |
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Author |
Bigiani, L.; Gasparotto, A.; Maccato, C.; Sada, C.; Verbeeck, J.; Andreu, T.; Morante, J.R.; Barreca, D. |
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Title |
Dual improvement of beta-MnO₂ oxygen evolution electrocatalysts via combined substrate control and surface engineering |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Chemcatchem |
Abbreviated Journal |
Chemcatchem |
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Volume |
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Issue |
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Pages |
1-10 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The development of catalysts with high intrinsic activity towards the oxygen evolution reaction (OER) plays a critical role in sustainable energy conversion and storage. Herein, we report on the development of efficient (photo)electrocatalysts based on functionalized MnO(2)systems. Specifically,beta-MnO(2)nanostructures grown by plasma enhanced-chemical vapor deposition on fluorine-doped tin oxide (FTO) or Ni foams were decorated with Co(3)O(4)or Fe(2)O(3)nanoparticles by radio frequency sputtering. Upon functionalization, FTO-supported materials yielded a performance increase with respect to bare MnO2, with current densities at 1.65 Vvs. the reversible hydrogen electrode (RHE) up to 3.0 and 3.5 mA/cm(2)in the dark and under simulated sunlight, respectively. On the other hand, the use of highly porous and conductive Ni foam substrates enabled to maximize cooperative interfacial effects between catalyst components. The best performing Fe2O3/MnO(2)system provided a current density of 17.9 mA/cm(2)at 1.65 Vvs. RHE, an overpotential as low as 390 mV, and a Tafel slope of 69 mV/decade under dark conditions, comparing favorably with IrO(2)and RuO(2)benchmarks. Overall, the control of beta-MnO2/substrate interactions and the simultaneous surface property engineering pave the way to an efficient energy generation from abundant natural resources. |
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Wos |
000571229000001 |
Publication Date |
2020-09-18 |
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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 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.5 |
Times cited |
5 |
Open Access |
Not_Open_Access |
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Notes |
; This work has been financially supported by Padova University DOR 2017-2019, P-DiSC #03BIRD2016-UNIPD and #03BIRD2018-UNIPD projects. A.G. acknowledges AMGA Foundation and INSTM Consortium. J.V. gratefully acknowledges funding from the GOA project “Solarpaint” of the University of Antwerp and the European Union's Horizon 2020 research and innovation programme under grant agreement No 823717-ESTEEM3. ; esteem3TA; esteem3reported |
Approved |
Most recent IF: 4.5; 2020 IF: 4.803 |
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Call Number |
UA @ admin @ c:irua:171949 |
Serial |
6493 |
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Author |
Bigiani, L.; Andreu, T.; Maccato, C.; Fois, E.; Gasparotto, A.; Sada, C.; Tabacchi, G.; Krishnan, D.; Verbeeck, J.; Ramon Morante, J.; Barreca, D. |
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Title |
Engineering Au/MnO₂ hierarchical nanoarchitectures for ethanol electrochemical valorization |
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 |
33 |
Pages |
16902-16907 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The design of eco-friendly electrocatalysts for ethanol valorization is an open challenge towards sustainable hydrogen production. Herein we present an original fabrication route to effective electrocatalysts for the ethanol oxidation reaction (EOR). In particular, hierarchical MnO(2)nanostructures are grown on high-area nickel foam scaffolds by a plasma-assisted strategy and functionalized with low amounts of optimally dispersed Au nanoparticles. This strategy leads to catalysts with a unique morphology, designed to enhance reactant-surface contacts and maximize active site utilization. The developed nanoarchitectures show superior performances for ethanol oxidation in alkaline media. We reveal that Au decoration boosts MnO(2)catalytic activity by inducing pre-dissociation and pre-oxidation of the adsorbed ethanol molecules. This evidence validates our strategy as an effective route for the development of green electrocatalysts for efficient electrical-to-chemical energy conversion. |
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Wos |
000562931300008 |
Publication Date |
2020-07-21 |
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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 |
16 |
Open Access |
OpenAccess |
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Notes |
; This work was financially supported by Padova University DOR 2016-2019 and P-DiSC #03BIRD2018-UNIPD OXYGENA projects, as well as by the INSTM Consortium (INSTMPD004 – NETTUNO), AMGA Foundation Mn4Energy project and Insubria University FAR2018. J. V. and D. K. acknowledge funding from the Flemish Government (Hercules), GOA project “Solarpaint” (Antwerp University) and European Union's H2020 programme under grant agreement no. 823717 ESTEEM3. The authors are grateful to Dr Gianluca Corr for skillful technical support. ; esteem3TA; esteem3reported |
Approved |
Most recent IF: 11.9; 2020 IF: 8.867 |
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Call Number |
UA @ admin @ c:irua:171989 |
Serial |
6506 |
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Author |
Barreca, D.; Gri, F.; Gasparotto, A.; Carraro, G.; Bigiani, L.; Altantzis, T.; Žener, B.; Lavrenčič Štangar, U.; Alessi, B.; Padmanaban, D.B.; Mariotti, D.; Maccato, C. |
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Title |
Multi-functional MnO2nanomaterials for photo-activated applications by a plasma-assisted fabrication route |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Nanoscale |
Abbreviated Journal |
Nanoscale |
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Volume |
11 |
Issue |
1 |
Pages |
98-108 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Supported MnO2-based nanomaterials were fabricated on fluorine-doped tin oxide substrates by plasma enhanced-chemical vapor deposition (PE-CVD) between 100 °C and 400 °C, starting from a fluorinated Mn(II) diamine diketonate precursor. Growth experiments yielded -MnO2 nanosystems with hierarchical morphology tuneable from dendritic structures to quasi-1D nanosystems as a function of growth temperature, whose variation enabled also a concomitant tailoring of the system fluorine content, and of the optical absorption and band gap. Preliminary photocatalytic tests were aimed at the investigation of photoinduced hydrophilic (PH) and solid phase photocatalytic (PC) performances of the present nanomaterials, as well as at the photodegradation of Plasmocorinth B azo-dye aqueous solutions. The obtained findings highlighted an attractive system photoactivity even under visible light, finely tailored by fluorine content, morphological organization and optical properties of the prepared nanostructures. The results indicate that the synthesized MnO2 nanosystems have potential applications as advanced smart materials for anti-fogging/self-cleaning end uses and water purification. |
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Wos |
000454327500037 |
Publication Date |
2018-10-10 |
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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 |
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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 |
7 |
Open Access |
OpenAccess |
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Notes |
Padova University DOR 2016–2017, P-DiSC #03BIRD2016-UNIPD projects, HERALD Cost Action MP1402 – 37831 and ACTION post-doc fellowship are acknowledged for financial support. T.A. acknowledges a post-doctoral grant from the Research Foundation Flanders (FWO). Thanks are also due to Prof. Sara Bals (EMAT, University of Antwerp, Belgium), Prof. Romana Cerc Korošec and to Dr. Lev Matoh (University of Ljubljana, Slovenia), and to Prof. Elza Bontempi (Brescia University, Italy). The work was also supported by EPSRC (award EP/R008841/1, EP/M024938/1). |
Approved |
Most recent IF: 7.367 |
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Call Number |
EMAT @ emat @UA @ admin @ c:irua:156388 |
Serial |
5148 |
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