{"title":"Unusually improved peracetic acid activation for ultrafast organic compound removal through redox-inert Mg incorporation into active Co3O4","authors":"Xiaoyang Li, Jiahang Liu, Yingying Chu, Mengying Qian, Zhichao Yang, Weiming Zhang","doi":"10.1016/j.apcatb.2024.124601","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.124601","url":null,"abstract":"Peracetic acid (PAA) is increasingly used in advanced oxidation processes (AOPs) for water purification, yet there remains a critical need for highly-efficient and low-cost activators. Here, we constructed abundant oxygen vacancies (OVs) into redox-active CoO by incorporating redox-inert Mg species (MgCoO), achieving ultrafast degradation of sulfamethoxazole (SMX) via PAA activation. The MgCoO/PAA system successfully degraded SMX within 3 min, with a removal rate 154.8 times higher than the CoO/PAA system, surpassing even previously reported single-atom catalysts. The primary active species identified was the acetylperoxyl radical (CHC(O)OO•), with Co-oxo acting as a secondary active species that produced O-labeled sulfone compounds. We proposed a novel mechanism involving redox-inert Mg species that simultaneously strengthened PAA adsorption and activation. The enriched surface hydroxyl groups after Mg incorporation elevated the affinity for PAA binding. Meanwhile, the reduced Co average valence state and enhanced electron transfer capability facilitated PAA activation. This study offers an in-depth knowledge of redox-inert alkaline earth metals in PAA-AOPs.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"38 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142250051","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yucong Miao, Zhenhua Li, Lan Luo, Wangsong Chen, Lili Ma, Kui Fan, Yingjie Song, Yaofeng Hu, Rengui Li, Mingfei Shao
{"title":"Photoelectrocatalytic allylic C–H oxidation to allylic alcohols coupled with hydrogen evolution","authors":"Yucong Miao, Zhenhua Li, Lan Luo, Wangsong Chen, Lili Ma, Kui Fan, Yingjie Song, Yaofeng Hu, Rengui Li, Mingfei Shao","doi":"10.1016/j.apcatb.2024.124588","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.124588","url":null,"abstract":"Allylic C–H bond oxidation of cycloolefins to allylic alcohols has attracted tremendous attention owing to its widespread application in pharmaceuticals production and natural synthesis. However, the production of allylic alcohols still suffers from the challenges of unsatisfactory selectivity and harsh conditions. Herein, we report the sustainable photoelectrocatalytic (PEC) allylic C–H oxidation to allylic alcohols, achieving the oxidation of cyclohexene to 2-cyclohexenol with a selectivity of 97.2 %. We reveal the reaction pathway wherein photogenerated holes and OH synergistically activate cyclohexene to carbocation intermediates, and these intermediates combine with OH to produce 2-cyclohexenol. Additionally, the mechanism by enriching OH in local area of photoanode surface to enhance PEC performance is uncovered. Furthermore, we designed a self-powered PEC reaction system, attaining a 2-cyclohexenol productivity of 11.95 μmol h (selectivity > 97 %) coupled with a H productivity of 1.44 mL h, demonstrating the application potential of this new strategy.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"23 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249988","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jindi Yang, Hanqing Yin, Aijun Du, Mike Tebyetekerwa, Chuanbiao Bie, Zhuyuan Wang, Zhimeng Sun, Zhongguo Zhang, Xiangkang Zeng, Xiwang Zhang
{"title":"Unveiling O2 adsorption on non-metallic active site for selective photocatalytic H2O2 production","authors":"Jindi Yang, Hanqing Yin, Aijun Du, Mike Tebyetekerwa, Chuanbiao Bie, Zhuyuan Wang, Zhimeng Sun, Zhongguo Zhang, Xiangkang Zeng, Xiwang Zhang","doi":"10.1016/j.apcatb.2024.124586","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.124586","url":null,"abstract":"Photocatalytic oxygen reduction reaction (ORR) offers a promising pathway for sustainable hydrogen peroxide (HO) production but faces challenges in developing catalysts with good ORR selectivity. Herein, we report that tailoring O adsorption on non-metallic active sites can optimize ORR selectivity. This concept is demonstrated on three carbon nitrides with different atomic configurations: polymeric carbon nitride (PCN), lithium-poly triazine imide (Li-PTI), and sodium-poly heptazine imide (Na-PHI). Na-PHI emerges as a strong candidate for HO production due to the end-on adsorption mode and suitable adsorption strength with O. Synthesized Na-PHI, PCN, and Li-PTI are characterized, with Na-PHI showing superior light absorption, charge carrier separation, and remarkable selectivity (92 %) for two-electron ORR. Consequently, Na-PHI achieves a high HO generation rate of 3.48 mmol g h, surpassing Li-PTI and PCN by 9.2 and 33 times, respectively. This study underscores the importance of O adsorption on non-metallic active sites for selective photocatalytic HO generation.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"112 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249989","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Junpeng Yue, Hanpei Yang, Lei Zhou, Chen Liu, Shi Wang, Xudong Kang
{"title":"At least five: Benefit origins of potassium and sodium co-doping on carbon nitride for integrating pharmaceuticals degradation and hydrogen peroxide production","authors":"Junpeng Yue, Hanpei Yang, Lei Zhou, Chen Liu, Shi Wang, Xudong Kang","doi":"10.1016/j.apcatb.2024.124599","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.124599","url":null,"abstract":"Benefit origins of potassium (K) and sodium (Na) co-doping on carbon nitride for integrating pharmaceutical degradation and hydrogen peroxide (HO) production was investigated. K and Na co-doped carbon nitride (CN-K/Na) with modified crystallinity and surface structure was synthesized by ionothermal polymerization of urea. The CN-K/Na exhibited an apparent quantum yield of 26.2 % in HO photosynthesis at 400 nm (isopropanol as proton donor), and it was better at extracting proton from pharmaceutical-laden wastewater to produce HO than pristine carbon nitride. These superior performances are attributed to the benefits directly or indirectly caused by the co-doping: i) Na optimizes in-plane charge transfer, ii) K builds channel for interplane charge transfer, iii) cyano group as Lewis acid site adsorbs and activates oxygen, iv) amino group as Lewis base site extracts and releases protons, v) increased visible-light absorption. This work offers significant insights into designing polymeric photocatalysts for environmental management and energy conservation.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"3 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142268114","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuanjun Hu, Guanhui Liu, Ting Song, Xiayi Hu, Bei Long, Guo-Jun Deng
{"title":"Single-atom Cu sites on covalent organic frameworks with Kagome lattices for visible-light-driven CO2 reduction to propylene","authors":"Yuanjun Hu, Guanhui Liu, Ting Song, Xiayi Hu, Bei Long, Guo-Jun Deng","doi":"10.1016/j.apcatb.2024.124587","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.124587","url":null,"abstract":"CO to multicarbon fuels via photocatalytic conversion, especially propylene, is a viable pathway, but propylene remains unreported due to the two C-C coupling with the eighteen-electron reduction process. Herein, [1,1′-biphenyl]-3,3′,5,5′-tetracarbaldehyde, and [2,2-bipyridine]-5,5-diamine units were condensed and synthesized in combination with a post-modification strategy, named BTA-COF-M (M = H, Cu, Fe, Co, Ni or Zn). BTA-COF-Cu has distinct kagome lattices and abundant exposed-atom Cu sites, which can induce CO to undergo two C-C couplings into CH products under visible light illumination. According to experimental and theoretical analyses, the outstanding performance of BTA-COF-Cu can be attributed to the ideal synergistic contribution of the Kagome lattices and the atomic Cu active sites, which promote CO adsorption/activation, facilitate photoexcited charge carrier dynamics, and induce secondary coupling of key intermediates. This research provides an innovative perspective for the construction of Kagome lattice COF with monatomic metal sites for CO reduction to high value-added propylene.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"15 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249992","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Qinyue Wu, Xinfei Fan, Kaiyuan Liu, Xie Quan, Yanming Liu
{"title":"Efficient and selective electroreduction of nitrate to ammonia via interfacial engineering of B-doped Cu nanoneedles","authors":"Qinyue Wu, Xinfei Fan, Kaiyuan Liu, Xie Quan, Yanming Liu","doi":"10.1016/j.apcatb.2024.124597","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.124597","url":null,"abstract":"Electrocatalytic nitrate reduction to ammonia is a promising method to mitigate nitrate contamination and produce valuable chemical. However, it still suffers from slow active hydrogen (*H) transfer kinetics and unfavorable thermodynamics. Here the *H transfer and reaction energy barrier of nitrate reduction reaction were regulated on B-doped Cu nanoneedles (Cu NNs-B) to enhance ammonia electrosynthesis via interfacial engineering. The high-curvature nanoneedles showed locally enhanced electric fields, which promoted *H supply from water dissociation. B-doping provided Cu/Cu active sites for the activation of nitrate and intermediates. Due to the simultaneously improved *H supply kinetics and reaction thermodynamics, Cu NNs-B was efficient for reducing nitrate to ammonia, achieving high Faradaic efficiencies (FEs) of 95.1–98.6 % and ammonia yields of 0.12–1.33 mmol·h·cm at 50–1500 mg·L NO-N. Nitrate was selectively converted to ammonia with the remaining nitrate and nitrite concentrations below drinking water standards. Experimental and DFT results revealed Cu NNs-B with properly higher nanotip curvature was more favorable for boosting ammonia electrosynthesis from both kinetics and thermodynamics.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"199 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249990","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jian Meng, Manfen Liang, Jinglin Mu, Zhichao Miao, Hong Huang, Ruirui Qi, Lechen Diao, Shuping Zhuo, Jin Zhou
{"title":"Regulating p-orbital electronic configuration of In2O3 by thickness-controlled carbon layer for efficient electrocatalytic CO2 reduction to HCOOH","authors":"Jian Meng, Manfen Liang, Jinglin Mu, Zhichao Miao, Hong Huang, Ruirui Qi, Lechen Diao, Shuping Zhuo, Jin Zhou","doi":"10.1016/j.apcatb.2024.124596","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.124596","url":null,"abstract":"As for developing efficient Indium (In)-based catalyst of CO reduction to HCOOH, the modulation of electronic structure stands as a pivotal factor. However, the precise control of -orbital electronic configuration of InO remains challenging. Herein, the carbon-coated InO (InO@C) with precisely controllable carbon thickness is developed. The InO modified by moderate carbon layer thickness exhibits an impressive FE exceeding 90 % and maintains a constant current density of 110 mA cm even after 100 h. Meanwhile, it achieves a FE of 97 % and a current of 550 mA in a membrane electrode assembly. The catalyst maintains satisfactory activity even under low CO concentration and acidic electrolytes. The density functional theory (DFT) calculations show that carbon layer successfully improves the -orbital electronic configuration of InO and perfects the adsorption energy of *OCHO intermediate. This work can provide a guidance for regulating electronic configuration and designing high-efficiency electrocatalyst.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"4 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249991","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}