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Identification of Dynamic Active Sites Among Cu Species Derived from MOFs@CuPc for Electrocatalytic Nitrate Reduction Reaction to Ammonia
Highlights Cu species with tunable loading supported on N-doped TiO 2 /C were successfully fabricated utilizing MOFs@CuPc precursors via the pre-anchor and post-pyrolysis strategy. Cu species with tunable loading supported on N-doped TiO 2 /C were successfully fabricated utilizing MOFs@CuPc precurso...
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Published in: | Nano-micro letters 2023-12, Vol.15 (1), p.110-110, Article 110 |
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Main Authors: | , , , , , , , |
Format: | Article |
Language: | English |
Subjects: | |
Citations: | Items that this one cites Items that cite this one |
Online Access: | Get full text |
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Summary: | Highlights
Cu species with tunable loading supported on N-doped TiO
2
/C were successfully fabricated utilizing MOFs@CuPc precursors via the pre-anchor and post-pyrolysis strategy.
Cu species with tunable loading supported on N-doped TiO
2
/C were successfully fabricated utilizing MOFs@CuPc precursors via the pre-anchor and post-pyrolysis strategy.
Restructured CuN
4
&Cu
4
performed the highest NH
3
yield (88.2 mmol h
−1
g
cata
−1
) and FE (~94.3%) at − 0.75 V due to optimal adsorption of NO
3
−
and rapid conversion of the key intermediates.
Direct electrochemical nitrate reduction reaction (NITRR) is a promising strategy to alleviate the unbalanced nitrogen cycle while achieving the electrosynthesis of ammonia. However, the restructuration of the high-activity Cu-based electrocatalysts in the NITRR process has hindered the identification of dynamical active sites and in-depth investigation of the catalytic mechanism. Herein, Cu species (single-atom, clusters, and nanoparticles) with tunable loading supported on N-doped TiO
2
/C are successfully manufactured with MOFs@CuPc precursors via the pre-anchor and post-pyrolysis strategy. Restructuration behavior among Cu species is co-dependent on the Cu loading and reaction potential, as evidenced by the advanced
operando
X-ray absorption spectroscopy, and there exists an incompletely reversible transformation of the restructured structure to the initial state. Notably, restructured CuN
4
&Cu
4
deliver the high NH
3
yield of 88.2 mmol h
−1
g
cata
−1
and FE (~ 94.3%) at − 0.75 V, resulting from the optimal adsorption of NO
3
−
as well as the rapid conversion of *NH
2
OH to *NH
2
intermediates originated from the modulation of charge distribution and
d
-band center for Cu site. This work not only uncovers CuN
4
&Cu
4
have the promising NITRR but also identifies the dynamic Cu species active sites that play a critical role in the efficient electrocatalytic reduction in nitrate to ammonia. |
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ISSN: | 2311-6706 2150-5551 |
DOI: | 10.1007/s40820-023-01091-9 |