Toward Visible-Light Photochemical CO2‑to-CH4 Conversion in Aqueous Solutions Using Sensitized Molecular Catalysis: Difference between revisions

Latest revision as of 14:36, 5 September 2024

A photochemical reduction of CO₂ was achieved using an iron porphyrin catalyst and an iridium complex as the photosensitizer. Carbon monoxide, produced with a TON of 178 under optimized conditions, was the main product, methane was produced in a substantial amount with the TON of 32, while hydrogen was formed as a minor byproduct. The experiments were performed under irradiation with λ > 420 nm in acetonitrile and in the presence of various amines as sacrificial electron donors.

Advances and special progress[edit | edit source]

The catalytic reduction of CO₂ could also be realized under aqueous conditions (acetonitrile/water 3:7 v:v), yielding carbon monoxide as the main product while methane was produced with selectivity up to 10% (TON of 3).

Additional remarks[edit | edit source]

Among the various amines employed as sacrificial electron donors, TEA appeared as the best choice to maximize CO₂ product formation.

Content of the published article in detail[edit | edit source]

The article contains results for the reduction of CO₂ to CO as the main product under visible-light irradiation using iron porphyrin complex Fe(pTMAPP)Cl₅ (Fe(pTMAPP)Cl5) as the catalysts, an iridium complex as the photosensitizer and various amines as the sacrificial electron donor. The catalytic system performs best (referring to the TON of CO production) with Ir(ppy)₃ (Ir(ppy)3) as the photosensitizer and TEA as the sacrificial electron donor.

Catalyst[edit | edit source]

Fe(pTMAPP)Cl5

Photosensitizer[edit | edit source]

[Ir(ppy)2(bpy)][PF6] Ir(ppy)3

Investigation[edit | edit source]

	cat	cat conc [µM]	PS	PS conc [mM]	e-D	e-D conc [M]	solvent A	additives	λexc [nm]	TON CO	TON CH4	TON H2
1.	Fe(pTMAPP)Cl5	0.002	[Ir(ppy)2(bpy)][PF6]	0.2	TEA	0.05	MeCN		> 420	178	32	103
2.	Fe(pTMAPP)Cl5	0.002	[Ir(ppy)2(bpy)][PF6]	0.2	TEOA	0.05	MeCN		> 420	134	23	67
3.	Fe(pTMAPP)Cl5	0.002	[Ir(ppy)2(bpy)][PF6]	0.2	DIPEA	0.05	MeCN		> 420	151	24	77
4.	Fe(pTMAPP)Cl5	0.002	[Ir(ppy)2(bpy)][PF6]	0.2	TEA	0.05	MeCN		> 420	24	3	5
5.	Fe(pTMAPP)Cl5	0.002	[Ir(ppy)2(bpy)][PF6]	0.2	TEOA	0.05	MeCN		> 420	19	3	4
6.	Fe(pTMAPP)Cl5	0.002	[Ir(ppy)2(bpy)][PF6]	0.2	DIPEA	0.05	MeCN		> 420	20	3	4
7.	Fe(pTMAPP)Cl5	0.002	Ir(ppy)3	0.2	TEA	0.05	MeCN		> 420	198	31	24
8.	Fe(pTMAPP)Cl5	0.002	Ir(ppy)3	0.2	TEA	0.05	MeCN		> 420		89	18
9.	Fe(pTMAPP)Cl5	0.002	Ir(ppy)3	0.2	TEA	0.05	MeCN	TFE	> 420		100	19
10.	Fe(pTMAPP)Cl5	0.002	Ir(ppy)3	0.2	TEA	0.05	MeCN	TFE	> 420		195	45

Investigation-Name: Photocatalytic reduction of CO2: conditions optimization

	analyte	anl conc [mM]	reduction potential	solvent	electrolyte	gas	WE	RE
1.	[Ir(ppy)2(bpy)][PF6]	0.5	-2.0 , -1.4	MeCN	TBAPF6	argon	glassy carbon	SCE
2.	[Ir(ppy)2(bpy)][PF6]	0.5	-2.0, -1.4	MeCN	TBAPF6	CO	glassy carbon	SCE
3.	[Ir(ppy)2(bpy)][PF6]	0.5	-2.0, -1.4	MeCN	TBAPF6	CO	glassy carbon	SCE
4.	[Ir(ppy)2(bpy)][PF6]	0.5	-2.0, -1.4	MeCN	TBAPF6	CO	glassy carbon	SCE
5.	[Ir(ppy)2(bpy)][PF6]	0.5	-2.0	MeCN	TBAPF6	CO	glassy carbon	SCE

The results show an increase in current when the solution is irradiated and triethylamine (TEA) is added (see condition column).

Investigation-Name: Cyclic voltammetry in various conditions

Sacrificial electron donor[edit | edit source]

In this study, the experiments were conducted with TEA (TEA), TEOA (TEOA), and DIPEA (DIPEA) as sacrificial electron donors.

Additives[edit | edit source]

In some experiments described in this study, TFE (TFE) was used as an additive.

Investigations

Cyclic voltammetry in various conditions (Assay, Cyclic Voltammetry experiments)
Photocatalytic reduction of CO2: conditions optimization (Molecular process, Photocatalytic CO2 conversion experiments)

DOI	10.1021/acs.jpcc.8b00950
Authors	Heng Rao, Julien Bonin, Marc Robert,
Submitted	28.04.2018
Published online	28.04.2018
Licenses	-
Subjects	Surfaces, Coatings and Films, Physical and Theoretical Chemistry, General Energy, Electronic, Optical and Magnetic Materials
Go to literature page

@@ Line 1: / Line 1: @@
 {{BaseTemplate}}
-{{#doiinfobox: 10.1021/acs.jpcc.8b00950}}
+{{DOI|doi=10.1021/acs.jpcc.8b00950}}
+=== Abstract ===
-==== Investigation ====
+==== Summary====
-{{#experimentlist:|form=Photocatalytic_CO2_conversion_experiments|name=Table 1}}
+A photochemical reduction of CO<sub>2</sub> was achieved using an iron porphyrin catalyst and an iridium complex as the photosensitizer. Carbon monoxide, produced with a TON of 178 under optimized conditions, was the main product, methane was produced in a substantial amount with the TON of 32, while hydrogen was formed as a minor byproduct. The experiments were performed under irradiation with ''λ >'' 420 nm in acetonitrile and in the presence of various amines as sacrificial electron donors.
-==== Catalyst ====
+==== Advances and special progress====
-{{#moleculelink:|link=NRVILUOLTIKJEU-NGWNFTKISA-I}}
+The catalytic reduction of CO<sub>2</sub> could also be realized under aqueous conditions (acetonitrile/water 3:7 v:v), yielding carbon monoxide as the main product while methane was produced with selectivity up to 10% (TON of 3).
-==== Photosensitizer ====
+==== Additional remarks====
-{{#moleculelink:|link=UEEXRMUCXBPYOV-UHFFFAOYSA-N}} <chemform smiles="C1C=C2C3C([Ir+]4(N5C(C6N4=CC=CC=6)=CC=CC=5)4(N5C(C6C4=CC=CC=6)=CC=CC=5)N2=CC=1)=CC=CC=3" inchi="1S/2C11H9N.C10H8N2.Ir/c2*1-2-6-10(7-3-1)11-8-4-5-9-12-11;1-3-7-11-9(5-1)10-6-2-4-8-12-10;/h2*1-9H;1-8H;/q;;;+1" inchikey="WEEPMIZXGXTKSO-UHFFFAOYSA-N" height="200px" width="300px" float="none">
+Among the various amines employed as sacrificial electron donors, TEA appeared as the best choice to maximize CO<sub>2</sub> product formation.
-   -INDIGO-01262315082D
+=== Content of the published article in detail ===
+The article contains results for the reduction of CO<sub>2</sub> to CO as the main product under visible-light irradiation using iron porphyrin complex Fe(pTMAPP)Cl<sub>5</sub> ({{#moleculelink:|link=LKNRTBVZMCBYCY-NGWNFTKISA-I|image=false|width=300|height=200}}) as the catalysts, an iridium complex as the photosensitizer and various amines as the sacrificial electron donor. The catalytic system performs best (referring to the TON of CO production) with Ir(ppy)<sub>3</sub> ({{#moleculelink: |link=NSABRUJKERBGOU-UHFFFAOYSA-N|image=false|width=300|height=200}}) as the photosensitizer and TEA as the sacrificial electron donor.
+==== Catalyst====
+{{#moleculelink:|link=LKNRTBVZMCBYCY-NGWNFTKISA-I|image=true|width=300|height=200}}
+====Photosensitizer====
+<chemform smiles="C1C=C[C-]2[Ir+3]3([C-]4C=CC=CC=4C4C=CC=CN=43)3(N4=CC=CC=C4C4C=CC=CN=43)N3=CC=CC=C3C=2C=1.[P-](F)(F)(F)(F)(F)F" inchi="1S/2C11H8N.C10H8N2.F6P.Ir/c2*1-2-6-10(7-3-1)11-8-4-5-9-12-11;1-3-7-11-9(5-1)10-6-2-4-8-12-10;1-7(2,3,4,5)6;/h2*1-6,8-9H;1-8H;;/q2*-1;;-1;+3" inchikey="RJJGJTKSOSSNNL-UHFFFAOYSA-N" height="200px" width="300px" float="none">
+   -INDIGO-08012317332D
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 </chemform>
+{{#moleculelink: |link=NSABRUJKERBGOU-UHFFFAOYSA-N|image=true}}
+====Investigation====
+{{#experimentlist: |form=Photocatalytic_CO2_conversion_experiments|name=Photocatalytic reduction of CO2: conditions optimization}}
+{{#experimentlist: |form=Cyclic_Voltammetry_experiments|name=Cyclic voltammetry in various conditions}}
+====Sacrificial electron donor====
+In this study, the experiments were conducted with TEA ({{#moleculelink:|link=ZMANZCXQSJIPKH-UHFFFAOYSA-N|image=false|width=300|height=200}}), TEOA ({{#moleculelink:|link=GSEJCLTVZPLZKY-UHFFFAOYSA-N|image=false|width=300|height=200}}), and DIPEA ({{#moleculelink:|link=JGFZNNIVVJXRND-UHFFFAOYSA-N|image=false|width=300|height=200}}) as sacrificial electron donors.
-==== Sacrificial electron donor ====
+====Additives====
-{{#moleculelink:|link=GSEJCLTVZPLZKY-UHFFFAOYSA-N}} {{#moleculelink:|link=ZMANZCXQSJIPKH-UHFFFAOYSA-N}} {{#moleculelink:|link=JGFZNNIVVJXRND-UHFFFAOYSA-N}}
+In some experiments described in this study, TFE ({{#moleculelink:|link=RHQDFWAXVIIEBN-UHFFFAOYSA-N|image=false|width=300|height=200}}) was used as an additive.
-[[Category:Photocatalytic conversion of CO2 to CH4]]
+[[Category:Photocatalytic CO2 conversion to CH4]][[Category:Publication]]

Toward Visible-Light Photochemical CO2‑to-CH4 Conversion in Aqueous Solutions Using Sensitized Molecular Catalysis: Difference between revisions

Latest revision as of 14:36, 5 September 2024

Contents

Abstract[edit | edit source]

Summary[edit | edit source]

Advances and special progress[edit | edit source]

Additional remarks[edit | edit source]

Content of the published article in detail[edit | edit source]

Catalyst[edit | edit source]

Photosensitizer[edit | edit source]

Investigation[edit | edit source]

Sacrificial electron donor[edit | edit source]

Additives[edit | edit source]

Investigations

Topics

Toward Visible-Light Photochemical CO2‑to-CH4 Conversion in Aqueous Solutions Using Sensitized Molecular Catalysis: Difference between revisions

Latest revision as of 14:36, 5 September 2024

Abstract[edit | edit source]

Summary[edit | edit source]

Advances and special progress[edit | edit source]

Additional remarks[edit | edit source]

Content of the published article in detail[edit | edit source]

Catalyst[edit | edit source]

Photosensitizer[edit | edit source]

Investigation[edit | edit source]

Sacrificial electron donor[edit | edit source]

Additives[edit | edit source]

Investigations

Current site

Topics