{"title":"饱和醇电催化氧化Ni-Co双金属氧化物具有平衡的B-和l -酸性活性位点","authors":"Junqing Ma, Wenshu Luo, Xunlu Wang, Xu Yu, Jiacheng Jayden Wang, Huashuai Hu, Hanxiao Du, Jianrong Zeng, Wei Chen, Minghui Yang, Jiacheng Wang, Xiangzhi Cui","doi":"10.1007/s40820-025-01893-z","DOIUrl":null,"url":null,"abstract":"<div><p>Investigating structural and hydroxyl group effects in electrooxidation of alcohols to value-added products by solid-acid electrocatalysts is essential for upgrading biomass alcohols. Herein, we report efficient electrocatalytic oxidations of saturated alcohols (C<sub>1</sub>-C<sub>6</sub>) to selectively form formate using NiCo hydroxide (NiCo–OH) derived NiCo<sub>2</sub>O<sub>4</sub> solid-acid electrocatalysts with balanced Lewis acid (LASs) and Brønsted acid sites (BASs). Thermal treatment transforms BASs-rich (89.6%) NiCo–OH into NiCo<sub>2</sub>O<sub>4</sub> with nearly equal distribution of LASs (53.1%) and BASs (46.9%) which synergistically promote adsorption and activation of OH<sup>−</sup> and alcohol molecules for enhanced oxidation activity. In contrast, BASs-enriched NiCo–OH facilitates formation of higher valence metal sites, beneficial for water oxidation. The combined experimental studies and theoretical calculation imply the oxidation ability of C<sub>1</sub>-C<sub>6</sub> alcohols increases as increased number of hydroxyl groups and decreased HOMO–LUMO gaps: methanol (C<sub>1</sub>) < ethylene glycol (C<sub>2</sub>) < glycerol (C<sub>3</sub>) < meso-erythritol (C<sub>4</sub>) < xylitol (C<sub>5</sub>) < sorbitol (C<sub>6</sub>), while the formate selectivity shows the opposite trend from 100 to 80%. This study unveils synergistic roles of LASs and BASs, as well as hydroxyl group effect in electro-upgrading of alcohols using solid-acid electrocatalysts.\n</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":714,"journal":{"name":"Nano-Micro Letters","volume":"18 1","pages":""},"PeriodicalIF":36.3000,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s40820-025-01893-z.pdf","citationCount":"0","resultStr":"{\"title\":\"Saturated Alcohols Electrocatalytic Oxidations on Ni-Co Bimetal Oxide Featuring Balanced B- and L-Acidic Active Sites\",\"authors\":\"Junqing Ma, Wenshu Luo, Xunlu Wang, Xu Yu, Jiacheng Jayden Wang, Huashuai Hu, Hanxiao Du, Jianrong Zeng, Wei Chen, Minghui Yang, Jiacheng Wang, Xiangzhi Cui\",\"doi\":\"10.1007/s40820-025-01893-z\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Investigating structural and hydroxyl group effects in electrooxidation of alcohols to value-added products by solid-acid electrocatalysts is essential for upgrading biomass alcohols. Herein, we report efficient electrocatalytic oxidations of saturated alcohols (C<sub>1</sub>-C<sub>6</sub>) to selectively form formate using NiCo hydroxide (NiCo–OH) derived NiCo<sub>2</sub>O<sub>4</sub> solid-acid electrocatalysts with balanced Lewis acid (LASs) and Brønsted acid sites (BASs). Thermal treatment transforms BASs-rich (89.6%) NiCo–OH into NiCo<sub>2</sub>O<sub>4</sub> with nearly equal distribution of LASs (53.1%) and BASs (46.9%) which synergistically promote adsorption and activation of OH<sup>−</sup> and alcohol molecules for enhanced oxidation activity. In contrast, BASs-enriched NiCo–OH facilitates formation of higher valence metal sites, beneficial for water oxidation. The combined experimental studies and theoretical calculation imply the oxidation ability of C<sub>1</sub>-C<sub>6</sub> alcohols increases as increased number of hydroxyl groups and decreased HOMO–LUMO gaps: methanol (C<sub>1</sub>) < ethylene glycol (C<sub>2</sub>) < glycerol (C<sub>3</sub>) < meso-erythritol (C<sub>4</sub>) < xylitol (C<sub>5</sub>) < sorbitol (C<sub>6</sub>), while the formate selectivity shows the opposite trend from 100 to 80%. This study unveils synergistic roles of LASs and BASs, as well as hydroxyl group effect in electro-upgrading of alcohols using solid-acid electrocatalysts.\\n</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":714,\"journal\":{\"name\":\"Nano-Micro Letters\",\"volume\":\"18 1\",\"pages\":\"\"},\"PeriodicalIF\":36.3000,\"publicationDate\":\"2025-08-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://link.springer.com/content/pdf/10.1007/s40820-025-01893-z.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nano-Micro Letters\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s40820-025-01893-z\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"Engineering\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nano-Micro Letters","FirstCategoryId":"88","ListUrlMain":"https://link.springer.com/article/10.1007/s40820-025-01893-z","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"Engineering","Score":null,"Total":0}
Saturated Alcohols Electrocatalytic Oxidations on Ni-Co Bimetal Oxide Featuring Balanced B- and L-Acidic Active Sites
Investigating structural and hydroxyl group effects in electrooxidation of alcohols to value-added products by solid-acid electrocatalysts is essential for upgrading biomass alcohols. Herein, we report efficient electrocatalytic oxidations of saturated alcohols (C1-C6) to selectively form formate using NiCo hydroxide (NiCo–OH) derived NiCo2O4 solid-acid electrocatalysts with balanced Lewis acid (LASs) and Brønsted acid sites (BASs). Thermal treatment transforms BASs-rich (89.6%) NiCo–OH into NiCo2O4 with nearly equal distribution of LASs (53.1%) and BASs (46.9%) which synergistically promote adsorption and activation of OH− and alcohol molecules for enhanced oxidation activity. In contrast, BASs-enriched NiCo–OH facilitates formation of higher valence metal sites, beneficial for water oxidation. The combined experimental studies and theoretical calculation imply the oxidation ability of C1-C6 alcohols increases as increased number of hydroxyl groups and decreased HOMO–LUMO gaps: methanol (C1) < ethylene glycol (C2) < glycerol (C3) < meso-erythritol (C4) < xylitol (C5) < sorbitol (C6), while the formate selectivity shows the opposite trend from 100 to 80%. This study unveils synergistic roles of LASs and BASs, as well as hydroxyl group effect in electro-upgrading of alcohols using solid-acid electrocatalysts.
期刊介绍：
Nano-Micro Letters is a peer-reviewed, international, interdisciplinary, and open-access journal published under the SpringerOpen brand.
Nano-Micro Letters focuses on the science, experiments, engineering, technologies, and applications of nano- or microscale structures and systems in various fields such as physics, chemistry, biology, material science, and pharmacy.It also explores the expanding interfaces between these fields.
Nano-Micro Letters particularly emphasizes the bottom-up approach in the length scale from nano to micro. This approach is crucial for achieving industrial applications in nanotechnology, as it involves the assembly, modification, and control of nanostructures on a microscale.
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