Controlled synthesis of MOF-derived hollow and yolk–shell nanocages for improved water oxidation and selective ethylene glycol reformation

Huang, M; Cao, C; Liu, L; Wei, W; Zhu, QL; Huang, Z

Controlled synthesis of MOF-derived hollow and yolk–shell nanocages for improved water oxidation and selective ethylene glycol reformation

Huang, M Cao, C Liu, L Wei, W Zhu, QL Huang, Z

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Publisher:: Elsevier BV
Publication Type:: Journal Article
Citation:: eScience, 2023, 3, (5), pp. 100118
Issue Date:: 2023-10-01

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Field	Value	Language
dc.contributor.author	Huang, M
dc.contributor.author	Cao, C
dc.contributor.author	Liu, L
dc.contributor.author	Wei, W
dc.contributor.author	Zhu, QL
dc.contributor.author	Huang, Z https://orcid.org/0000-0003-1985-0884
dc.date.accessioned	2023-11-08T23:02:17Z
dc.date.available	2023-11-08T23:02:17Z
dc.date.issued	2023-10-01
dc.identifier.citation	eScience, 2023, 3, (5), pp. 100118
dc.identifier.issn	2667-1417
dc.identifier.issn	2667-1417
dc.identifier.uri	http://hdl.handle.net/10453/173251
dc.description.abstract	Delicately designed metal–organic framework (MOF)-derived nanostructured electrocatalysts are essential for improving the reaction kinetics of the oxygen evolution reaction and tuning the selectivity of small organic molecule oxidation reactions. Herein, novel oxalate-modified hollow CoFe-based layered double hydroxide nanocages (h-CoFe-LDH NCs) and yolk–shell ZIF@CoFe-LDH nanocages (ys-ZIF@CoFe-LDH NCs) are developed through an etching–doping reconstruction strategy from a Co-based MOF precursor (ZIF-67). The distinctive nanostructures, along with the incorporation of the secondary metal element and intercalated oxalate groups, enable h-CoFe-LDH NCs and ys-ZIF@CoFe-LDH NCs to expose more active sites with high intrinsic activity. The resultant h-CoFe-LDH NCs exhibit outstanding OER activity with an overpotential of only 278 mV to deliver a current density of 50 mA cm−2. Additionally, controlling the reconstruction degree enables the formation of ys-ZIF@CoFe-LDH NCs with a yolk–shell nanocage nanostructure, which show outstanding electrocatalytic performance for the selective ethylene glycol oxidation reaction (EGOR) toward formate, with a Faradaic efficiency of up to 91%. Consequently, a hybrid water electrolysis system integrating the EGOR and the hydrogen evolution reaction using Pt/C\|\|ys-ZIF@CoFe-LDH NCs is explored for energy-saving hydrogen production, requiring a cell voltage 127 mV lower than water electrolysis to achieve a current density of 50 mA cm−2. This work demonstrates a feasible way to design advanced MOF-derived electrocatalysts toward enhanced electrocatalytic reactions.
dc.language	en
dc.publisher	Elsevier BV
dc.relation	http://purl.org/au-research/grants/arc/FT190100658
dc.relation	http://purl.org/au-research/grants/arc/DP220103458
dc.relation.ispartof	eScience
dc.relation.isbasedon	10.1016/j.esci.2023.100118
dc.rights	info:eu-repo/semantics/restrictedAccess
dc.title	Controlled synthesis of MOF-derived hollow and yolk–shell nanocages for improved water oxidation and selective ethylene glycol reformation
dc.type	Journal Article
utslib.citation.volume	3
pubs.organisational-group	/University of Technology Sydney
pubs.organisational-group	/University of Technology Sydney/Faculty of Engineering and Information Technology
pubs.organisational-group	/University of Technology Sydney/Faculty of Engineering and Information Technology/School of Civil and Environmental Engineering
pubs.organisational-group	/University of Technology Sydney/Strength - CTWW - Centre for Technology in Water and Wastewater Treatment
utslib.copyright.status	recently_added	*
dc.date.updated	2023-11-08T23:02:15Z
pubs.issue	5
pubs.publication-status	Published
pubs.volume	3
utslib.citation.issue	5

Abstract:

Delicately designed metal–organic framework (MOF)-derived nanostructured electrocatalysts are essential for improving the reaction kinetics of the oxygen evolution reaction and tuning the selectivity of small organic molecule oxidation reactions. Herein, novel oxalate-modified hollow CoFe-based layered double hydroxide nanocages (h-CoFe-LDH NCs) and yolk–shell ZIF@CoFe-LDH nanocages (ys-ZIF@CoFe-LDH NCs) are developed through an etching–doping reconstruction strategy from a Co-based MOF precursor (ZIF-67). The distinctive nanostructures, along with the incorporation of the secondary metal element and intercalated oxalate groups, enable h-CoFe-LDH NCs and ys-ZIF@CoFe-LDH NCs to expose more active sites with high intrinsic activity. The resultant h-CoFe-LDH NCs exhibit outstanding OER activity with an overpotential of only 278 mV to deliver a current density of 50 mA cm−2. Additionally, controlling the reconstruction degree enables the formation of ys-ZIF@CoFe-LDH NCs with a yolk–shell nanocage nanostructure, which show outstanding electrocatalytic performance for the selective ethylene glycol oxidation reaction (EGOR) toward formate, with a Faradaic efficiency of up to 91%. Consequently, a hybrid water electrolysis system integrating the EGOR and the hydrogen evolution reaction using Pt/C||ys-ZIF@CoFe-LDH NCs is explored for energy-saving hydrogen production, requiring a cell voltage 127 mV lower than water electrolysis to achieve a current density of 50 mA cm−2. This work demonstrates a feasible way to design advanced MOF-derived electrocatalysts toward enhanced electrocatalytic reactions.

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http://hdl.handle.net/10453/173251