Defect-phase engineered NiTi-TiO2 enabling near-unity selective photocatalytic CO2-to-methanol conversion

Abstract Scaling up methanol yields by artificial photosynthesis at a modest cost remains thermodynamically challenge. Designing concerted reaction sites to control intermediate evolution and stimulate proton-coupled electron transfer (PCET) is necessary. Here we show a nickel-titanium-based catalys...

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Main Authors: Ruonan Wang, Mingjia Zhang, Jingjing Liu, Xu Wu, Shule Zhang, Qin Zhong, Jianfeng Yao
Format: Article
Language:English
Published: Nature Portfolio 2025-08-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-63179-7
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author Ruonan Wang
Mingjia Zhang
Jingjing Liu
Xu Wu
Shule Zhang
Qin Zhong
Jianfeng Yao
author_facet Ruonan Wang
Mingjia Zhang
Jingjing Liu
Xu Wu
Shule Zhang
Qin Zhong
Jianfeng Yao
author_sort Ruonan Wang
collection DOAJ
description Abstract Scaling up methanol yields by artificial photosynthesis at a modest cost remains thermodynamically challenge. Designing concerted reaction sites to control intermediate evolution and stimulate proton-coupled electron transfer (PCET) is necessary. Here we show a nickel-titanium-based catalyst that achieves near-millimolar hourly methanol yields with 99.79% selectivity and a solar-to-chemical conversion efficiency of 2.23%. This catalyst is synthesized through one-step etching of NiTi-layered double hydroxide, which generates abundant unsaturated sites, along with the in-situ formation of amorphous TiO2. Revealed by in-situ characterizations, these defect-rich units effectively suppress the formation of undesirable carbonate while promoting the favorable *COOH intermediate. Furthermore, theoretical simulations confirm this *COOH boost facilitates the production of *CO and accelerates the PCET steps. This work significantly advances efficient methanol production by artificial photosynthesis and offers fundamental insights into controlling reaction pathways for renewable fuel synthesis.
format Article
id doaj-art-848da321f79f476792c0723185dcc047
institution Kabale University
issn 2041-1723
language English
publishDate 2025-08-01
publisher Nature Portfolio
record_format Article
series Nature Communications
spelling doaj-art-848da321f79f476792c0723185dcc0472025-08-24T11:39:36ZengNature PortfolioNature Communications2041-17232025-08-0116111210.1038/s41467-025-63179-7Defect-phase engineered NiTi-TiO2 enabling near-unity selective photocatalytic CO2-to-methanol conversionRuonan Wang0Mingjia Zhang1Jingjing Liu2Xu Wu3Shule Zhang4Qin Zhong5Jianfeng Yao6Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, College of Chemical Engineering, Nanjing Forestry UniversityCollege of Chemistry and Chemical Engineering, Nanjing University of Science and TechnologyCollege of Chemistry and Chemical Engineering, Nanjing University of Science and TechnologyCollege of Chemistry and Chemical Engineering, Taiyuan University of TechnologyCollege of Chemistry and Chemical Engineering, Nanjing University of Science and TechnologyCollege of Chemistry and Chemical Engineering, Nanjing University of Science and TechnologyJiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, College of Chemical Engineering, Nanjing Forestry UniversityAbstract Scaling up methanol yields by artificial photosynthesis at a modest cost remains thermodynamically challenge. Designing concerted reaction sites to control intermediate evolution and stimulate proton-coupled electron transfer (PCET) is necessary. Here we show a nickel-titanium-based catalyst that achieves near-millimolar hourly methanol yields with 99.79% selectivity and a solar-to-chemical conversion efficiency of 2.23%. This catalyst is synthesized through one-step etching of NiTi-layered double hydroxide, which generates abundant unsaturated sites, along with the in-situ formation of amorphous TiO2. Revealed by in-situ characterizations, these defect-rich units effectively suppress the formation of undesirable carbonate while promoting the favorable *COOH intermediate. Furthermore, theoretical simulations confirm this *COOH boost facilitates the production of *CO and accelerates the PCET steps. This work significantly advances efficient methanol production by artificial photosynthesis and offers fundamental insights into controlling reaction pathways for renewable fuel synthesis.https://doi.org/10.1038/s41467-025-63179-7
spellingShingle Ruonan Wang
Mingjia Zhang
Jingjing Liu
Xu Wu
Shule Zhang
Qin Zhong
Jianfeng Yao
Defect-phase engineered NiTi-TiO2 enabling near-unity selective photocatalytic CO2-to-methanol conversion
Nature Communications
title Defect-phase engineered NiTi-TiO2 enabling near-unity selective photocatalytic CO2-to-methanol conversion
title_full Defect-phase engineered NiTi-TiO2 enabling near-unity selective photocatalytic CO2-to-methanol conversion
title_fullStr Defect-phase engineered NiTi-TiO2 enabling near-unity selective photocatalytic CO2-to-methanol conversion
title_full_unstemmed Defect-phase engineered NiTi-TiO2 enabling near-unity selective photocatalytic CO2-to-methanol conversion
title_short Defect-phase engineered NiTi-TiO2 enabling near-unity selective photocatalytic CO2-to-methanol conversion
title_sort defect phase engineered niti tio2 enabling near unity selective photocatalytic co2 to methanol conversion
url https://doi.org/10.1038/s41467-025-63179-7
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AT mingjiazhang defectphaseengineerednititio2enablingnearunityselectivephotocatalyticco2tomethanolconversion
AT jingjingliu defectphaseengineerednititio2enablingnearunityselectivephotocatalyticco2tomethanolconversion
AT xuwu defectphaseengineerednititio2enablingnearunityselectivephotocatalyticco2tomethanolconversion
AT shulezhang defectphaseengineerednititio2enablingnearunityselectivephotocatalyticco2tomethanolconversion
AT qinzhong defectphaseengineerednititio2enablingnearunityselectivephotocatalyticco2tomethanolconversion
AT jianfengyao defectphaseengineerednititio2enablingnearunityselectivephotocatalyticco2tomethanolconversion