Photoelectrocatalytic H2 evolution from integrated photocatalysts adsorbed on NiO

A new approach to increasing the faradaic efficiency of dye-sensitised photocathodes for H 2 evolution from water, using integrated photocatalysts, furnished with ester groups on the peripheral ligands, [Ru(decb) 2 (bpt)PdCl(H 2 O)](PF 6 ) 2 ( 1 ) and [Ru(decb) 2 (2,5-bpp)PtI(CH 3 CN)](PF 6 ) 2 ( 2...

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Published in:	Chemical science (Cambridge) Vol. 10; no. 1; pp. 99 - 112
Main Authors:	Põldme, Nils, O'Reilly, Laura, Fletcher, Ian, Portoles, Jose, Sazanovich, Igor V., Towrie, Michael, Long, Conor, Vos, Johannes G., Pryce, Mary T., Gibson, Elizabeth A.
Format:	Journal Article
Language:	English
Published:	Cambridge Royal Society of Chemistry 2019
Subjects:	Catalysis Chemistry Chromophores Hydrogen evolution Light irradiation Nickel oxides Photocatalysis Photocatalysts Photocathodes Photoelectric effect Photoelectric emission Ruthenium Silver chloride Surface analysis (chemical) White light
ISSN:	2041-6520, 2041-6539
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Abstract	A new approach to increasing the faradaic efficiency of dye-sensitised photocathodes for H 2 evolution from water, using integrated photocatalysts, furnished with ester groups on the peripheral ligands, [Ru(decb) 2 (bpt)PdCl(H 2 O)](PF 6 ) 2 ( 1 ) and [Ru(decb) 2 (2,5-bpp)PtI(CH 3 CN)](PF 6 ) 2 ( 2 ), (decb = 4,4′-diethylcarboxy-2,2′-bipyridine, bpp = 2,2':5′,2′′-terpyridine, bpt = 3,5-bis(2-pyridyl)-1,2,4-triazole) is described. Overall, 1 \|NiO is superior to previously reported photocathodes, producing photocurrent densities of 30–35 μA cm −2 at an applied bias of −0.2 V vs. Ag/AgCl over 1 hour of continuous white light irradiation, resulting in the generation of 0.41 μmol h −1 cm −2 of H 2 with faradaic efficiencies of up to 90%. Furthermore, surface analysis of the photocathodes before and after photoelectrocatalysis revealed that the ruthenium bipyridyl chromophore and Pd catalytic centre ( 1 ) were photochemically stable, highlighting the benefits of the approach towards robust, hybrid solar-to-fuel devices.
AbstractList	A new approach to increasing the faradaic efficiency of dye-sensitised photocathodes for H 2 evolution from water, using integrated photocatalysts, furnished with ester groups on the peripheral ligands, [Ru(decb) 2 (bpt)PdCl(H 2 O)](PF 6 ) 2 ( 1 ) and [Ru(decb) 2 (2,5-bpp)PtI(CH 3 CN)](PF 6 ) 2 ( 2 ), (decb = 4,4′-diethylcarboxy-2,2′-bipyridine, bpp = 2,2':5′,2′′-terpyridine, bpt = 3,5-bis(2-pyridyl)-1,2,4-triazole) is described. Overall, 1 \|NiO is superior to previously reported photocathodes, producing photocurrent densities of 30–35 μA cm −2 at an applied bias of −0.2 V vs. Ag/AgCl over 1 hour of continuous white light irradiation, resulting in the generation of 0.41 μmol h −1 cm −2 of H 2 with faradaic efficiencies of up to 90%. Furthermore, surface analysis of the photocathodes before and after photoelectrocatalysis revealed that the ruthenium bipyridyl chromophore and Pd catalytic centre ( 1 ) were photochemically stable, highlighting the benefits of the approach towards robust, hybrid solar-to-fuel devices. A new approach to increasing the faradaic efficiency of dye-sensitised photocathodes for H2 evolution from water is described, using integrated photocatalysts based on a ruthenium 4,4′-diethoxycarboxy-2,2′-bipyridine chromophore linked via terpyridine or triazole to a Pd or Pt-based H+ reduction catalyst. A new approach to increasing the faradaic efficiency of dye-sensitised photocathodes for H2 evolution from water, using integrated photocatalysts, furnished with ester groups on the peripheral ligands, [Ru(decb)2(bpt)PdCl(H2O)](PF6)2 (1) and [Ru(decb)2(2,5-bpp)PtI(CH3CN)](PF6)2 (2), (decb = 4,4′-diethylcarboxy-2,2′-bipyridine, bpp = 2,2':5′,2′′-terpyridine, bpt = 3,5-bis(2-pyridyl)-1,2,4-triazole) is described. Overall, 1\|NiO is superior to previously reported photocathodes, producing photocurrent densities of 30–35 μA cm–2 at an applied bias of –0.2 V vs. Ag/AgCl over 1 hour of continuous white light irradiation, resulting in the generation of 0.41 μmol h–1 cm–2 of H2 with faradaic efficiencies of up to 90%. Furthermore, surface analysis of the photocathodes before and after photoelectrocatalysis revealed that the ruthenium bipyridyl chromophore and Pd catalytic centre (1) were photochemically stable, highlighting the benefits of the approach towards robust, hybrid solar-to-fuel devices. A new approach to increasing the faradaic efficiency of dye-sensitised photocathodes for H2 evolution from water, using integrated photocatalysts, furnished with ester groups on the peripheral ligands, [Ru(decb)2(bpt)PdCl(H2O)](PF6)2 (1) and [Ru(decb)2(2,5-bpp)PtI(CH3CN)](PF6)2 (2), (decb = 4,4′-diethylcarboxy-2,2′-bipyridine, bpp = 2,2':5′,2′′-terpyridine, bpt = 3,5-bis(2-pyridyl)-1,2,4-triazole) is described. Overall, 1\|NiO is superior to previously reported photocathodes, producing photocurrent densities of 30–35 μA cm−2 at an applied bias of −0.2 V vs. Ag/AgCl over 1 hour of continuous white light irradiation, resulting in the generation of 0.41 μmol h−1 cm−2 of H2 with faradaic efficiencies of up to 90%. Furthermore, surface analysis of the photocathodes before and after photoelectrocatalysis revealed that the ruthenium bipyridyl chromophore and Pd catalytic centre (1) were photochemically stable, highlighting the benefits of the approach towards robust, hybrid solar-to-fuel devices. A new approach to increasing the faradaic efficiency of dye-sensitised photocathodes for H2 evolution from water, using integrated photocatalysts, furnished with ester groups on the peripheral ligands, [Ru(decb)2(bpt)PdCl(H2O)](PF6)2 (1) and [Ru(decb)2(2,5-bpp)PtI(CH3CN)](PF6)2 (2), (decb = 4,4'-diethylcarboxy-2,2'-bipyridine, bpp = 2,2':5',2''-terpyridine, bpt = 3,5-bis(2-pyridyl)-1,2,4-triazole) is described. Overall, 1\|NiO is superior to previously reported photocathodes, producing photocurrent densities of 30-35 μA cm-2 at an applied bias of -0.2 V vs. Ag/AgCl over 1 hour of continuous white light irradiation, resulting in the generation of 0.41 μmol h-1 cm-2 of H2 with faradaic efficiencies of up to 90%. Furthermore, surface analysis of the photocathodes before and after photoelectrocatalysis revealed that the ruthenium bipyridyl chromophore and Pd catalytic centre (1) were photochemically stable, highlighting the benefits of the approach towards robust, hybrid solar-to-fuel devices.A new approach to increasing the faradaic efficiency of dye-sensitised photocathodes for H2 evolution from water, using integrated photocatalysts, furnished with ester groups on the peripheral ligands, [Ru(decb)2(bpt)PdCl(H2O)](PF6)2 (1) and [Ru(decb)2(2,5-bpp)PtI(CH3CN)](PF6)2 (2), (decb = 4,4'-diethylcarboxy-2,2'-bipyridine, bpp = 2,2':5',2''-terpyridine, bpt = 3,5-bis(2-pyridyl)-1,2,4-triazole) is described. Overall, 1\|NiO is superior to previously reported photocathodes, producing photocurrent densities of 30-35 μA cm-2 at an applied bias of -0.2 V vs. Ag/AgCl over 1 hour of continuous white light irradiation, resulting in the generation of 0.41 μmol h-1 cm-2 of H2 with faradaic efficiencies of up to 90%. Furthermore, surface analysis of the photocathodes before and after photoelectrocatalysis revealed that the ruthenium bipyridyl chromophore and Pd catalytic centre (1) were photochemically stable, highlighting the benefits of the approach towards robust, hybrid solar-to-fuel devices.
Author	Pryce, Mary T. Vos, Johannes G. Portoles, Jose Põldme, Nils Fletcher, Ian Long, Conor Towrie, Michael O'Reilly, Laura Sazanovich, Igor V. Gibson, Elizabeth A.
AuthorAffiliation	a School of Natural and Environmental Science , Newcastle University , Newcastle upon Tyne , NE1 7RU , UK . Email: Elizabeth.gibson@ncl.ac.uk b School of Chemical Sciences , Dublin City University , Dublin 9 , Ireland . Email: Mary.pryce@dcu.ie c NEXUS XPS Laboratory , Newcastle University , Stephenson Building , Newcastle upon Tyne , NE1 7RU , UK . Email: nexus@ncl.ac.uk d Central Laser Facility , Research Complex at Harwell , STFC Rutherford Appleton Laboratory , Harwell Campus , Didcot , Oxfordshire OX11 0QX , UK . Email: Igor.Sazanovich@stfc.ac.uk
AuthorAffiliation_xml	– name: b School of Chemical Sciences , Dublin City University , Dublin 9 , Ireland . Email: Mary.pryce@dcu.ie – name: a School of Natural and Environmental Science , Newcastle University , Newcastle upon Tyne , NE1 7RU , UK . Email: Elizabeth.gibson@ncl.ac.uk – name: c NEXUS XPS Laboratory , Newcastle University , Stephenson Building , Newcastle upon Tyne , NE1 7RU , UK . Email: nexus@ncl.ac.uk – name: d Central Laser Facility , Research Complex at Harwell , STFC Rutherford Appleton Laboratory , Harwell Campus , Didcot , Oxfordshire OX11 0QX , UK . Email: Igor.Sazanovich@stfc.ac.uk
Author_xml	– sequence: 1 givenname: Nils surname: Põldme fullname: Põldme, Nils organization: School of Natural and Environmental Science, Newcastle University, Newcastle upon Tyne, UK – sequence: 2 givenname: Laura surname: O'Reilly fullname: O'Reilly, Laura organization: School of Chemical Sciences, Dublin City University, Dublin 9, Ireland – sequence: 3 givenname: Ian surname: Fletcher fullname: Fletcher, Ian organization: NEXUS XPS Laboratory, Newcastle University, Newcastle upon Tyne, UK – sequence: 4 givenname: Jose surname: Portoles fullname: Portoles, Jose organization: NEXUS XPS Laboratory, Newcastle University, Newcastle upon Tyne, UK – sequence: 5 givenname: Igor V. surname: Sazanovich fullname: Sazanovich, Igor V. organization: Central Laser Facility, Research Complex at Harwell, STFC Rutherford Appleton Laboratory, Didcot, UK – sequence: 6 givenname: Michael surname: Towrie fullname: Towrie, Michael organization: Central Laser Facility, Research Complex at Harwell, STFC Rutherford Appleton Laboratory, Didcot, UK – sequence: 7 givenname: Conor surname: Long fullname: Long, Conor organization: School of Chemical Sciences, Dublin City University, Dublin 9, Ireland – sequence: 8 givenname: Johannes G. surname: Vos fullname: Vos, Johannes G. organization: School of Chemical Sciences, Dublin City University, Dublin 9, Ireland – sequence: 9 givenname: Mary T. surname: Pryce fullname: Pryce, Mary T. organization: School of Chemical Sciences, Dublin City University, Dublin 9, Ireland – sequence: 10 givenname: Elizabeth A. orcidid: 0000-0002-6032-343X surname: Gibson fullname: Gibson, Elizabeth A. organization: School of Natural and Environmental Science, Newcastle University, Newcastle upon Tyne, UK
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Snippet	A new approach to increasing the faradaic efficiency of dye-sensitised photocathodes for H 2 evolution from water, using integrated photocatalysts, furnished... A new approach to increasing the faradaic efficiency of dye-sensitised photocathodes for H2 evolution from water, using integrated photocatalysts, furnished... A new approach to increasing the faradaic efficiency of dye-sensitised photocathodes for H2 evolution from water is described, using integrated photocatalysts...
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SubjectTerms	Catalysis Chemistry Chromophores Hydrogen evolution Light irradiation Nickel oxides Photocatalysis Photocatalysts Photocathodes Photoelectric effect Photoelectric emission Ruthenium Silver chloride Surface analysis (chemical) White light
Title	Photoelectrocatalytic H2 evolution from integrated photocatalysts adsorbed on NiO
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