---
_id: '12237'
abstract:
- lang: eng
text: Thermoelectric technology requires synthesizing complex materials where not
only the crystal structure but also other structural features such as defects,
grain size and orientation, and interfaces must be controlled. To date, conventional
solid-state techniques are unable to provide this level of control. Herein, we
present a synthetic approach in which dense inorganic thermoelectric materials
are produced by the consolidation of well-defined nanoparticle powders. The idea
is that controlling the characteristics of the powder allows the chemical transformations
that take place during consolidation to be guided, ultimately yielding inorganic
solids with targeted features. Different from conventional methods, syntheses
in solution can produce particles with unprecedented control over their size,
shape, crystal structure, composition, and surface chemistry. However, to date,
most works have focused only on the low-cost benefits of this strategy. In this
perspective, we first cover the opportunities that solution processing of the
powder offers, emphasizing the potential structural features that can be controlled
by precisely engineering the inorganic core of the particle, the surface, and
the organization of the particles before consolidation. We then discuss the challenges
of this synthetic approach and more practical matters related to solution processing.
Finally, we suggest some good practices for adequate knowledge transfer and improving
reproducibility among different laboratories.
acknowledgement: This work was financially supported by ISTA and the Werner Siemens
Foundation. M.C. has received funding from the European Union’s Horizon 2020 research
and innovation program under the Marie Skłodowska-Curie Grant Agreement no. 665385.
article_processing_charge: Yes (via OA deal)
article_type: original
author:
- first_name: Christine
full_name: Fiedler, Christine
id: bd3fceba-dc74-11ea-a0a7-c17f71817366
last_name: Fiedler
- first_name: Tobias
full_name: Kleinhanns, Tobias
id: 8BD9DE16-AB3C-11E9-9C8C-2A03E6697425
last_name: Kleinhanns
- first_name: Maria
full_name: Garcia, Maria
id: 6e5c50b8-97dc-11ed-be98-b0a74c84cae0
last_name: Garcia
- first_name: Seungho
full_name: Lee, Seungho
id: BB243B88-D767-11E9-B658-BC13E6697425
last_name: Lee
orcid: 0000-0002-6962-8598
- first_name: Mariano
full_name: Calcabrini, Mariano
id: 45D7531A-F248-11E8-B48F-1D18A9856A87
last_name: Calcabrini
- first_name: Maria
full_name: Ibáñez, Maria
id: 43C61214-F248-11E8-B48F-1D18A9856A87
last_name: Ibáñez
orcid: 0000-0001-5013-2843
citation:
ama: 'Fiedler C, Kleinhanns T, Garcia M, Lee S, Calcabrini M, Ibáñez M. Solution-processed
inorganic thermoelectric materials: Opportunities and challenges. Chemistry
of Materials. 2022;34(19):8471-8489. doi:10.1021/acs.chemmater.2c01967'
apa: 'Fiedler, C., Kleinhanns, T., Garcia, M., Lee, S., Calcabrini, M., & Ibáñez,
M. (2022). Solution-processed inorganic thermoelectric materials: Opportunities
and challenges. Chemistry of Materials. American Chemical Society. https://doi.org/10.1021/acs.chemmater.2c01967'
chicago: 'Fiedler, Christine, Tobias Kleinhanns, Maria Garcia, Seungho Lee, Mariano
Calcabrini, and Maria Ibáñez. “Solution-Processed Inorganic Thermoelectric Materials:
Opportunities and Challenges.” Chemistry of Materials. American Chemical
Society, 2022. https://doi.org/10.1021/acs.chemmater.2c01967.'
ieee: 'C. Fiedler, T. Kleinhanns, M. Garcia, S. Lee, M. Calcabrini, and M. Ibáñez,
“Solution-processed inorganic thermoelectric materials: Opportunities and challenges,”
Chemistry of Materials, vol. 34, no. 19. American Chemical Society, pp.
8471–8489, 2022.'
ista: 'Fiedler C, Kleinhanns T, Garcia M, Lee S, Calcabrini M, Ibáñez M. 2022. Solution-processed
inorganic thermoelectric materials: Opportunities and challenges. Chemistry of
Materials. 34(19), 8471–8489.'
mla: 'Fiedler, Christine, et al. “Solution-Processed Inorganic Thermoelectric Materials:
Opportunities and Challenges.” Chemistry of Materials, vol. 34, no. 19,
American Chemical Society, 2022, pp. 8471–89, doi:10.1021/acs.chemmater.2c01967.'
short: C. Fiedler, T. Kleinhanns, M. Garcia, S. Lee, M. Calcabrini, M. Ibáñez, Chemistry
of Materials 34 (2022) 8471–8489.
date_created: 2023-01-16T09:51:26Z
date_published: 2022-09-20T00:00:00Z
date_updated: 2023-08-04T09:38:26Z
day: '20'
ddc:
- '540'
department:
- _id: MaIb
doi: 10.1021/acs.chemmater.2c01967
ec_funded: 1
external_id:
isi:
- '000917837600001'
pmid:
- '36248227'
file:
- access_level: open_access
checksum: f7143e44ab510519d1949099c3558532
content_type: application/pdf
creator: dernst
date_created: 2023-01-30T07:35:09Z
date_updated: 2023-01-30T07:35:09Z
file_id: '12434'
file_name: 2022_ChemistryMaterials_Fiedler.pdf
file_size: 10923495
relation: main_file
success: 1
file_date_updated: 2023-01-30T07:35:09Z
has_accepted_license: '1'
intvolume: ' 34'
isi: 1
issue: '19'
keyword:
- Materials Chemistry
- General Chemical Engineering
- General Chemistry
language:
- iso: eng
month: '09'
oa: 1
oa_version: Published Version
page: 8471-8489
pmid: 1
project:
- _id: 2564DBCA-B435-11E9-9278-68D0E5697425
call_identifier: H2020
grant_number: '665385'
name: International IST Doctoral Program
publication: Chemistry of Materials
publication_identifier:
eissn:
- 1520-5002
issn:
- 0897-4756
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
related_material:
record:
- id: '12885'
relation: dissertation_contains
status: public
scopus_import: '1'
status: public
title: 'Solution-processed inorganic thermoelectric materials: Opportunities and challenges'
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8
volume: 34
year: '2022'
...
---
_id: '11705'
abstract:
- lang: eng
text: 'The broad implementation of thermoelectricity requires high-performance and
low-cost materials. One possibility is employing surfactant-free solution synthesis
to produce nanopowders. We propose the strategy of functionalizing “naked” particles’
surface by inorganic molecules to control the nanostructure and, consequently,
thermoelectric performance. In particular, we use bismuth thiolates to functionalize
surfactant-free SnTe particles’ surfaces. Upon thermal processing, bismuth thiolates
decomposition renders SnTe-Bi2S3 nanocomposites with synergistic functions: 1)
carrier concentration optimization by Bi doping; 2) Seebeck coefficient enhancement
and bipolar effect suppression by energy filtering; and 3) lattice thermal conductivity
reduction by small grain domains, grain boundaries and nanostructuration. Overall,
the SnTe-Bi2S3 nanocomposites exhibit peak z T up to 1.3 at 873 K and an average
z T of ≈0.6 at 300–873 K, which is among the highest reported for solution-processed
SnTe.'
acknowledged_ssus:
- _id: EM-Fac
- _id: NanoFab
acknowledgement: This research was supported by the Scientific Service Units (SSU)
of IST Austria through resources provided by Electron Microscopy Facility (EMF)
and the Nanofabrication Facility (NNF). This work was financially supported by IST
Austria and the Werner Siemens Foundation. C.C. acknowledges funding from the FWF
“Lise Meitner Fellowship” grant agreement M 2889-N. Lise Meitner Project (M2889-N).
Y.L. acknowledges funding from the European Union's Horizon 2020 research and innovation
program under the Marie Sklodowska-Curie grant agreement No. 754411. R.L.B. thanks
the National Science Foundation for support under DMR-1904719. MCS acknowledge MINECO
Juan de la Cierva Incorporation fellowship (JdlCI 2019) and Severo Ochoa. M.C.S.
and J.A. acknowledge funding from Generalitat de Catalunya 2017 SGR 327. ICN2 is
supported by the Severo Ochoa program from Spanish MINECO (Grant no. SEV-2017-0706)
and is funded by the CERCA Programme/Generalitat de Catalunya. This study was supported
by MCIN with funding from European Union NextGenerationEU (PRTR-C17.I1) and Generalitat
de Catalunya.
article_number: e202207002
article_processing_charge: Yes (via OA deal)
article_type: original
author:
- first_name: Cheng
full_name: Chang, Cheng
id: 9E331C2E-9F27-11E9-AE48-5033E6697425
last_name: Chang
orcid: 0000-0002-9515-4277
- first_name: Yu
full_name: Liu, Yu
id: 2A70014E-F248-11E8-B48F-1D18A9856A87
last_name: Liu
orcid: 0000-0001-7313-6740
- first_name: Seungho
full_name: Lee, Seungho
id: BB243B88-D767-11E9-B658-BC13E6697425
last_name: Lee
orcid: 0000-0002-6962-8598
- first_name: Maria
full_name: Spadaro, Maria
last_name: Spadaro
- first_name: Kristopher M.
full_name: Koskela, Kristopher M.
last_name: Koskela
- first_name: Tobias
full_name: Kleinhanns, Tobias
id: 8BD9DE16-AB3C-11E9-9C8C-2A03E6697425
last_name: Kleinhanns
- first_name: Tommaso
full_name: Costanzo, Tommaso
id: D93824F4-D9BA-11E9-BB12-F207E6697425
last_name: Costanzo
orcid: 0000-0001-9732-3815
- first_name: Jordi
full_name: Arbiol, Jordi
last_name: Arbiol
- first_name: Richard L.
full_name: Brutchey, Richard L.
last_name: Brutchey
- first_name: Maria
full_name: Ibáñez, Maria
id: 43C61214-F248-11E8-B48F-1D18A9856A87
last_name: Ibáñez
orcid: 0000-0001-5013-2843
citation:
ama: 'Chang C, Liu Y, Lee S, et al. Surface functionalization of surfactant-free
particles: A strategy to tailor the properties of nanocomposites for enhanced
thermoelectric performance. Angewandte Chemie - International Edition.
2022;61(35). doi:10.1002/anie.202207002'
apa: 'Chang, C., Liu, Y., Lee, S., Spadaro, M., Koskela, K. M., Kleinhanns, T.,
… Ibáñez, M. (2022). Surface functionalization of surfactant-free particles: A
strategy to tailor the properties of nanocomposites for enhanced thermoelectric
performance. Angewandte Chemie - International Edition. Wiley. https://doi.org/10.1002/anie.202207002'
chicago: 'Chang, Cheng, Yu Liu, Seungho Lee, Maria Spadaro, Kristopher M. Koskela,
Tobias Kleinhanns, Tommaso Costanzo, Jordi Arbiol, Richard L. Brutchey, and Maria
Ibáñez. “Surface Functionalization of Surfactant-Free Particles: A Strategy to
Tailor the Properties of Nanocomposites for Enhanced Thermoelectric Performance.”
Angewandte Chemie - International Edition. Wiley, 2022. https://doi.org/10.1002/anie.202207002.'
ieee: 'C. Chang et al., “Surface functionalization of surfactant-free particles:
A strategy to tailor the properties of nanocomposites for enhanced thermoelectric
performance,” Angewandte Chemie - International Edition, vol. 61, no. 35.
Wiley, 2022.'
ista: 'Chang C, Liu Y, Lee S, Spadaro M, Koskela KM, Kleinhanns T, Costanzo T, Arbiol
J, Brutchey RL, Ibáñez M. 2022. Surface functionalization of surfactant-free particles:
A strategy to tailor the properties of nanocomposites for enhanced thermoelectric
performance. Angewandte Chemie - International Edition. 61(35), e202207002.'
mla: 'Chang, Cheng, et al. “Surface Functionalization of Surfactant-Free Particles:
A Strategy to Tailor the Properties of Nanocomposites for Enhanced Thermoelectric
Performance.” Angewandte Chemie - International Edition, vol. 61, no. 35,
e202207002, Wiley, 2022, doi:10.1002/anie.202207002.'
short: C. Chang, Y. Liu, S. Lee, M. Spadaro, K.M. Koskela, T. Kleinhanns, T. Costanzo,
J. Arbiol, R.L. Brutchey, M. Ibáñez, Angewandte Chemie - International Edition
61 (2022).
date_created: 2022-07-31T22:01:48Z
date_published: 2022-08-26T00:00:00Z
date_updated: 2023-08-03T12:23:52Z
day: '26'
ddc:
- '540'
department:
- _id: MaIb
- _id: EM-Fac
doi: 10.1002/anie.202207002
ec_funded: 1
external_id:
isi:
- '000828274200001'
file:
- access_level: open_access
checksum: ad601f2b9e26e46ab4785162be58b5ed
content_type: application/pdf
creator: dernst
date_created: 2023-02-02T08:01:00Z
date_updated: 2023-02-02T08:01:00Z
file_id: '12476'
file_name: 2022_AngewandteChemieInternat_Chang.pdf
file_size: 4072650
relation: main_file
success: 1
file_date_updated: 2023-02-02T08:01:00Z
has_accepted_license: '1'
intvolume: ' 61'
isi: 1
issue: '35'
language:
- iso: eng
month: '08'
oa: 1
oa_version: Published Version
project:
- _id: 9B8804FC-BA93-11EA-9121-9846C619BF3A
grant_number: M02889
name: Bottom-up Engineering for Thermoelectric Applications
- _id: 260C2330-B435-11E9-9278-68D0E5697425
call_identifier: H2020
grant_number: '754411'
name: ISTplus - Postdoctoral Fellowships
publication: Angewandte Chemie - International Edition
publication_identifier:
eissn:
- 1521-3773
issn:
- 1433-7851
publication_status: published
publisher: Wiley
quality_controlled: '1'
scopus_import: '1'
status: public
title: 'Surface functionalization of surfactant-free particles: A strategy to tailor
the properties of nanocomposites for enhanced thermoelectric performance'
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8
volume: 61
year: '2022'
...
---
_id: '9118'
abstract:
- lang: eng
text: Cesium lead halides have intrinsically unstable crystal lattices and easily
transform within perovskite and nonperovskite structures. In this work, we explore
the conversion of the perovskite CsPbBr3 into Cs4PbBr6 in the presence of PbS
at 450 °C to produce doped nanocrystal-based composites with embedded Cs4PbBr6
nanoprecipitates. We show that PbBr2 is extracted from CsPbBr3 and diffuses into
the PbS lattice with a consequent increase in the concentration of free charge
carriers. This new doping strategy enables the adjustment of the density of charge
carriers between 1019 and 1020 cm–3, and it may serve as a general strategy for
doping other nanocrystal-based semiconductors.
acknowledgement: "M.C. has received funding from the European Union’s Horizon 2020
research and innovation programme under the Marie Skłodowska-Curie Grant Agreement
No. 665385. ICN2\r\nacknowledges funding from Generalitat de Catalunya 2017 SGR
327. ICN2 is supported by the Severo Ochoa program from Spanish MINECO (Grant No.
SEV-2017-0706) and is funded by the CERCA Programme/Generalitat de Catalunya. This
project has received funding from the European Union’s Horizon 2020 research and
innovation programme under grant agreement No 823717 − ESTEEM3. M.V.K. acknowledges
the support by the European Research Council under the Horizon 2020 Framework Program
(ERC Consolidator Grant SCALEHALO\r\nGrant Agreement No. 819740) and by FET-OPEN
project no. 862656 (DROP-IT)."
article_processing_charge: Yes (via OA deal)
article_type: original
author:
- first_name: Mariano
full_name: Calcabrini, Mariano
id: 45D7531A-F248-11E8-B48F-1D18A9856A87
last_name: Calcabrini
- first_name: Aziz
full_name: Genc, Aziz
last_name: Genc
- first_name: Yu
full_name: Liu, Yu
id: 2A70014E-F248-11E8-B48F-1D18A9856A87
last_name: Liu
orcid: 0000-0001-7313-6740
- first_name: Tobias
full_name: Kleinhanns, Tobias
id: 8BD9DE16-AB3C-11E9-9C8C-2A03E6697425
last_name: Kleinhanns
- first_name: Seungho
full_name: Lee, Seungho
id: BB243B88-D767-11E9-B658-BC13E6697425
last_name: Lee
orcid: 0000-0002-6962-8598
- first_name: Dmitry N.
full_name: Dirin, Dmitry N.
last_name: Dirin
- first_name: Quinten A.
full_name: Akkerman, Quinten A.
last_name: Akkerman
- first_name: Maksym V.
full_name: Kovalenko, Maksym V.
last_name: Kovalenko
- first_name: Jordi
full_name: Arbiol, Jordi
last_name: Arbiol
- first_name: Maria
full_name: Ibáñez, Maria
id: 43C61214-F248-11E8-B48F-1D18A9856A87
last_name: Ibáñez
orcid: 0000-0001-5013-2843
citation:
ama: Calcabrini M, Genc A, Liu Y, et al. Exploiting the lability of metal halide
perovskites for doping semiconductor nanocomposites. ACS Energy Letters.
2021;6(2):581-587. doi:10.1021/acsenergylett.0c02448
apa: Calcabrini, M., Genc, A., Liu, Y., Kleinhanns, T., Lee, S., Dirin, D. N., …
Ibáñez, M. (2021). Exploiting the lability of metal halide perovskites for doping
semiconductor nanocomposites. ACS Energy Letters. American Chemical Society.
https://doi.org/10.1021/acsenergylett.0c02448
chicago: Calcabrini, Mariano, Aziz Genc, Yu Liu, Tobias Kleinhanns, Seungho Lee,
Dmitry N. Dirin, Quinten A. Akkerman, Maksym V. Kovalenko, Jordi Arbiol, and Maria
Ibáñez. “Exploiting the Lability of Metal Halide Perovskites for Doping Semiconductor
Nanocomposites.” ACS Energy Letters. American Chemical Society, 2021. https://doi.org/10.1021/acsenergylett.0c02448.
ieee: M. Calcabrini et al., “Exploiting the lability of metal halide perovskites
for doping semiconductor nanocomposites,” ACS Energy Letters, vol. 6, no.
2. American Chemical Society, pp. 581–587, 2021.
ista: Calcabrini M, Genc A, Liu Y, Kleinhanns T, Lee S, Dirin DN, Akkerman QA, Kovalenko
MV, Arbiol J, Ibáñez M. 2021. Exploiting the lability of metal halide perovskites
for doping semiconductor nanocomposites. ACS Energy Letters. 6(2), 581–587.
mla: Calcabrini, Mariano, et al. “Exploiting the Lability of Metal Halide Perovskites
for Doping Semiconductor Nanocomposites.” ACS Energy Letters, vol. 6, no.
2, American Chemical Society, 2021, pp. 581–87, doi:10.1021/acsenergylett.0c02448.
short: M. Calcabrini, A. Genc, Y. Liu, T. Kleinhanns, S. Lee, D.N. Dirin, Q.A. Akkerman,
M.V. Kovalenko, J. Arbiol, M. Ibáñez, ACS Energy Letters 6 (2021) 581–587.
date_created: 2021-02-14T23:01:14Z
date_published: 2021-01-20T00:00:00Z
date_updated: 2023-08-07T13:46:00Z
day: '20'
ddc:
- '540'
department:
- _id: MaIb
doi: 10.1021/acsenergylett.0c02448
ec_funded: 1
external_id:
isi:
- '000619803400036'
file:
- access_level: open_access
checksum: 6fa7374bf8b95fdfe6e6c595322a6689
content_type: application/pdf
creator: dernst
date_created: 2021-02-17T07:36:52Z
date_updated: 2021-02-17T07:36:52Z
file_id: '9155'
file_name: 2021_ACSEnergyLetters_Calcabrini.pdf
file_size: 5071201
relation: main_file
success: 1
file_date_updated: 2021-02-17T07:36:52Z
has_accepted_license: '1'
intvolume: ' 6'
isi: 1
issue: '2'
language:
- iso: eng
month: '01'
oa: 1
oa_version: Published Version
page: 581-587
project:
- _id: 2564DBCA-B435-11E9-9278-68D0E5697425
call_identifier: H2020
grant_number: '665385'
name: International IST Doctoral Program
publication: ACS Energy Letters
publication_identifier:
eissn:
- 2380-8195
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
related_material:
record:
- id: '12885'
relation: dissertation_contains
status: public
scopus_import: '1'
status: public
title: Exploiting the lability of metal halide perovskites for doping semiconductor
nanocomposites
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8
volume: 6
year: '2021'
...
---
_id: '10123'
abstract:
- lang: eng
text: Solution synthesis of particles emerged as an alternative to prepare thermoelectric
materials with less demanding processing conditions than conventional solid-state
synthetic methods. However, solution synthesis generally involves the presence
of additional molecules or ions belonging to the precursors or added to enable
solubility and/or regulate nucleation and growth. These molecules or ions can
end up in the particles as surface adsorbates and interfere in the material properties.
This work demonstrates that ionic adsorbates, in particular Na⁺ ions, are electrostatically
adsorbed in SnSe particles synthesized in water and play a crucial role not only
in directing the material nano/microstructure but also in determining the transport
properties of the consolidated material. In dense pellets prepared by sintering
SnSe particles, Na remains within the crystal lattice as dopant, in dislocations,
precipitates, and forming grain boundary complexions. These results highlight
the importance of considering all the possible unintentional impurities to establish
proper structure-property relationships and control material properties in solution-processed
thermoelectric materials.
acknowledged_ssus:
- _id: EM-Fac
- _id: NanoFab
acknowledgement: 'Y.L. and M.C. contributed equally to this work. This research was
supported by the Scientific Service Units (SSU) of IST Austria through resources
provided by Electron Microscopy Facility (EMF) and the Nanofabrication Facility
(NNF). This work was financially supported by IST Austria and the Werner Siemens
Foundation. Y.L. acknowledges funding from the European Union''s Horizon 2020 research
and innovation program under the Marie Sklodowska-Curie grant agreement No. 754411.
M.C. has received funding from the European Union''s Horizon 2020 research and innovation
program under the Marie Skłodowska-Curie Grant Agreement No. 665385. Y.Y. and O.C.-M.
acknowledge the financial support from DFG within the project SFB 917: Nanoswitches.
J.L. is a Serra Húnter Fellow and is grateful to ICREA Academia program. C.C. acknowledges
funding from the FWF “Lise Meitner Fellowship” grant agreement M 2889-N.'
article_number: '2106858'
article_processing_charge: Yes (via OA deal)
article_type: original
author:
- first_name: Yu
full_name: Liu, Yu
id: 2A70014E-F248-11E8-B48F-1D18A9856A87
last_name: Liu
orcid: 0000-0001-7313-6740
- first_name: Mariano
full_name: Calcabrini, Mariano
id: 45D7531A-F248-11E8-B48F-1D18A9856A87
last_name: Calcabrini
orcid: 0000-0003-4566-5877
- first_name: Yuan
full_name: Yu, Yuan
last_name: Yu
- first_name: Aziz
full_name: Genç, Aziz
last_name: Genç
- first_name: Cheng
full_name: Chang, Cheng
id: 9E331C2E-9F27-11E9-AE48-5033E6697425
last_name: Chang
orcid: 0000-0002-9515-4277
- first_name: Tommaso
full_name: Costanzo, Tommaso
id: D93824F4-D9BA-11E9-BB12-F207E6697425
last_name: Costanzo
orcid: 0000-0001-9732-3815
- first_name: Tobias
full_name: Kleinhanns, Tobias
id: 8BD9DE16-AB3C-11E9-9C8C-2A03E6697425
last_name: Kleinhanns
- first_name: Seungho
full_name: Lee, Seungho
id: BB243B88-D767-11E9-B658-BC13E6697425
last_name: Lee
orcid: 0000-0002-6962-8598
- first_name: Jordi
full_name: Llorca, Jordi
last_name: Llorca
- first_name: Oana
full_name: Cojocaru‐Mirédin, Oana
last_name: Cojocaru‐Mirédin
- first_name: Maria
full_name: Ibáñez, Maria
id: 43C61214-F248-11E8-B48F-1D18A9856A87
last_name: Ibáñez
orcid: 0000-0001-5013-2843
citation:
ama: 'Liu Y, Calcabrini M, Yu Y, et al. The importance of surface adsorbates in
solution‐processed thermoelectric materials: The case of SnSe. Advanced Materials.
2021;33(52). doi:10.1002/adma.202106858'
apa: 'Liu, Y., Calcabrini, M., Yu, Y., Genç, A., Chang, C., Costanzo, T., … Ibáñez,
M. (2021). The importance of surface adsorbates in solution‐processed thermoelectric
materials: The case of SnSe. Advanced Materials. Wiley. https://doi.org/10.1002/adma.202106858'
chicago: 'Liu, Yu, Mariano Calcabrini, Yuan Yu, Aziz Genç, Cheng Chang, Tommaso
Costanzo, Tobias Kleinhanns, et al. “The Importance of Surface Adsorbates in Solution‐processed
Thermoelectric Materials: The Case of SnSe.” Advanced Materials. Wiley,
2021. https://doi.org/10.1002/adma.202106858.'
ieee: 'Y. Liu et al., “The importance of surface adsorbates in solution‐processed
thermoelectric materials: The case of SnSe,” Advanced Materials, vol. 33,
no. 52. Wiley, 2021.'
ista: 'Liu Y, Calcabrini M, Yu Y, Genç A, Chang C, Costanzo T, Kleinhanns T, Lee
S, Llorca J, Cojocaru‐Mirédin O, Ibáñez M. 2021. The importance of surface adsorbates
in solution‐processed thermoelectric materials: The case of SnSe. Advanced Materials.
33(52), 2106858.'
mla: 'Liu, Yu, et al. “The Importance of Surface Adsorbates in Solution‐processed
Thermoelectric Materials: The Case of SnSe.” Advanced Materials, vol. 33,
no. 52, 2106858, Wiley, 2021, doi:10.1002/adma.202106858.'
short: Y. Liu, M. Calcabrini, Y. Yu, A. Genç, C. Chang, T. Costanzo, T. Kleinhanns,
S. Lee, J. Llorca, O. Cojocaru‐Mirédin, M. Ibáñez, Advanced Materials 33 (2021).
date_created: 2021-10-11T20:07:24Z
date_published: 2021-12-29T00:00:00Z
date_updated: 2023-08-14T07:25:27Z
day: '29'
ddc:
- '620'
department:
- _id: EM-Fac
- _id: MaIb
doi: 10.1002/adma.202106858
ec_funded: 1
external_id:
isi:
- '000709899300001'
pmid:
- '34626034'
file:
- access_level: open_access
checksum: 990bccc527c64d85cf1c97885110b5f4
content_type: application/pdf
creator: cchlebak
date_created: 2022-02-03T13:16:14Z
date_updated: 2022-02-03T13:16:14Z
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file_name: 2021_AdvancedMaterials_Liu.pdf
file_size: 5595666
relation: main_file
success: 1
file_date_updated: 2022-02-03T13:16:14Z
has_accepted_license: '1'
intvolume: ' 33'
isi: 1
issue: '52'
keyword:
- mechanical engineering
- mechanics of materials
- general materials science
language:
- iso: eng
month: '12'
oa: 1
oa_version: Published Version
pmid: 1
project:
- _id: 2564DBCA-B435-11E9-9278-68D0E5697425
call_identifier: H2020
grant_number: '665385'
name: International IST Doctoral Program
- _id: 260C2330-B435-11E9-9278-68D0E5697425
call_identifier: H2020
grant_number: '754411'
name: ISTplus - Postdoctoral Fellowships
- _id: 9B8804FC-BA93-11EA-9121-9846C619BF3A
grant_number: M02889
name: Bottom-up Engineering for Thermoelectric Applications
- _id: 9B8F7476-BA93-11EA-9121-9846C619BF3A
name: 'HighTE: The Werner Siemens Laboratory for the High Throughput Discovery of
Semiconductors for Waste Heat Recovery'
publication: Advanced Materials
publication_identifier:
eissn:
- 1521-4095
issn:
- 0935-9648
publication_status: published
publisher: Wiley
quality_controlled: '1'
related_material:
record:
- id: '12885'
relation: dissertation_contains
status: public
scopus_import: '1'
status: public
title: 'The importance of surface adsorbates in solution‐processed thermoelectric
materials: The case of SnSe'
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8
volume: 33
year: '2021'
...
---
_id: '8189'
abstract:
- lang: eng
text: Direct ethanol fuel cells (DEFCs) show a huge potential to power future electric
vehicles and portable electronics, but their deployment is currently limited by
the unavailability of proper electrocatalysis for the ethanol oxidation reaction
(EOR). In this work, we engineer a new electrocatalyst by incorporating phosphorous
into a palladium-tin alloy and demonstrate a significant performance improvement
toward EOR. We first detail a synthetic method to produce Pd2Sn:P nanocrystals
that incorporate 35% of phosphorus. These nanoparticles are supported on carbon
black and tested for EOR. Pd2Sn:P/C catalysts exhibit mass current densities up
to 5.03 A mgPd−1, well above those of Pd2Sn/C, PdP2/C and Pd/C reference catalysts.
Furthermore, a twofold lower Tafel slope and a much longer durability are revealed
for the Pd2Sn:P/C catalyst compared with Pd/C. The performance improvement is
rationalized with the aid of density functional theory (DFT) calculations considering
different phosphorous chemical environments. Depending on its oxidation state,
surface phosphorus introduces sites with low energy OH− adsorption and/or strongly
influences the electronic structure of palladium and tin to facilitate the oxidation
of the acetyl to acetic acid, which is considered the EOR rate limiting step.
DFT calculations also points out that the durability improvement of Pd2Sn:P/C
catalyst is associated to the promotion of OH adsorption that accelerates the
oxidation of intermediate poisoning COads, reactivating the catalyst surface.
acknowledgement: This work was supported by the European Regional Development Funds
and by the Spanish Ministerio de Economía y Competitividad through the project SEHTOP,
ENE2016- 77798-C4-3-R, and ENE2017-85087-C3. X. Y. thanks the China Scholarship
Council for the scholarship support. J. Liu acknowledges support from the Jiangsu
University Foundation (4111510011). J. Li obtained International Postdoctoral Exchange
Fellowship Program (Talent-Introduction program) in 2019 and is grateful for the
project (2019M663468) funded by the China Postdoctoral Science Foundation. Authors
acknowledge funding from Generalitat de Catalunya 2017 SGR 327 and 2017 SGR 1246,
and from IST Austria. ICN2 acknowledges the support from the Severo Ochoa Programme
(MINECO, grant no. SEV-2017-0706) and is funded by the CERCA Programme/Generalitat
de Catalunya. J. Llorca is a Serra Húnter Fellow and is grateful to MICINN/FEDER
RTI2018-093996-B-C31, GC 2017 SGR 128 and to ICREA Academia program.
article_number: '105116'
article_processing_charge: No
article_type: original
author:
- first_name: Xiaoting
full_name: Yu, Xiaoting
last_name: Yu
- first_name: Junfeng
full_name: Liu, Junfeng
last_name: Liu
- first_name: Junshan
full_name: Li, Junshan
last_name: Li
- first_name: Zhishan
full_name: Luo, Zhishan
last_name: Luo
- first_name: Yong
full_name: Zuo, Yong
last_name: Zuo
- first_name: Congcong
full_name: Xing, Congcong
last_name: Xing
- first_name: Jordi
full_name: Llorca, Jordi
last_name: Llorca
- first_name: Déspina
full_name: Nasiou, Déspina
last_name: Nasiou
- first_name: Jordi
full_name: Arbiol, Jordi
last_name: Arbiol
- first_name: Kai
full_name: Pan, Kai
last_name: Pan
- first_name: Tobias
full_name: Kleinhanns, Tobias
id: 8BD9DE16-AB3C-11E9-9C8C-2A03E6697425
last_name: Kleinhanns
- first_name: Ying
full_name: Xie, Ying
last_name: Xie
- first_name: Andreu
full_name: Cabot, Andreu
last_name: Cabot
citation:
ama: Yu X, Liu J, Li J, et al. Phosphorous incorporation in Pd2Sn alloys for electrocatalytic
ethanol oxidation. Nano Energy. 2020;77(11). doi:10.1016/j.nanoen.2020.105116
apa: Yu, X., Liu, J., Li, J., Luo, Z., Zuo, Y., Xing, C., … Cabot, A. (2020). Phosphorous
incorporation in Pd2Sn alloys for electrocatalytic ethanol oxidation. Nano
Energy. Elsevier. https://doi.org/10.1016/j.nanoen.2020.105116
chicago: Yu, Xiaoting, Junfeng Liu, Junshan Li, Zhishan Luo, Yong Zuo, Congcong
Xing, Jordi Llorca, et al. “Phosphorous Incorporation in Pd2Sn Alloys for Electrocatalytic
Ethanol Oxidation.” Nano Energy. Elsevier, 2020. https://doi.org/10.1016/j.nanoen.2020.105116.
ieee: X. Yu et al., “Phosphorous incorporation in Pd2Sn alloys for electrocatalytic
ethanol oxidation,” Nano Energy, vol. 77, no. 11. Elsevier, 2020.
ista: Yu X, Liu J, Li J, Luo Z, Zuo Y, Xing C, Llorca J, Nasiou D, Arbiol J, Pan
K, Kleinhanns T, Xie Y, Cabot A. 2020. Phosphorous incorporation in Pd2Sn alloys
for electrocatalytic ethanol oxidation. Nano Energy. 77(11), 105116.
mla: Yu, Xiaoting, et al. “Phosphorous Incorporation in Pd2Sn Alloys for Electrocatalytic
Ethanol Oxidation.” Nano Energy, vol. 77, no. 11, 105116, Elsevier, 2020,
doi:10.1016/j.nanoen.2020.105116.
short: X. Yu, J. Liu, J. Li, Z. Luo, Y. Zuo, C. Xing, J. Llorca, D. Nasiou, J. Arbiol,
K. Pan, T. Kleinhanns, Y. Xie, A. Cabot, Nano Energy 77 (2020).
date_created: 2020-08-02T22:00:57Z
date_published: 2020-11-01T00:00:00Z
date_updated: 2023-08-22T08:24:05Z
day: '01'
department:
- _id: MaIb
doi: 10.1016/j.nanoen.2020.105116
external_id:
isi:
- '000581738300030'
intvolume: ' 77'
isi: 1
issue: '11'
language:
- iso: eng
month: '11'
oa_version: None
publication: Nano Energy
publication_identifier:
issn:
- 2211-2855
publication_status: published
publisher: Elsevier
quality_controlled: '1'
scopus_import: '1'
status: public
title: Phosphorous incorporation in Pd2Sn alloys for electrocatalytic ethanol oxidation
type: journal_article
user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8
volume: 77
year: '2020'
...