{"title":"Surface-bonded water in h-BN for synergistically triggering catalytic activity to hydrogen generation from ammonia borane via coordination dissociation","authors":"Huanhuan Zhang, Shuling Liu, Ruofan Shen, Saima Ashraf, Sehrish Mehdi, Shuyan Guan, Yanping Fan, Zhikun Peng, Jianchun Jiang, Baozhong Liu, Yongfeng Wang, Yanyan Liu, Baojun Li","doi":"10.1016/j.apcatb.2025.125729","DOIUrl":"https://doi.org/10.1016/j.apcatb.2025.125729","url":null,"abstract":"Developing catalysts with efficient activity to the reaction systems with water dissociation represents a significant and challenging mission in chemistry. Herein, CoP nanosheets supported on h-BN with surface-bonded water (CoP/h-BN OH ) is designed through a P-inducing strategy to stimulate the activity toward hydrogen generation. Hydroxyl functional groups (−OH) binds to B sites preferentially on h-BN surface during the process of surface hydroxylation to form B OH . The P-inducing strategy modulates the electronic configuration nearby Co and combines with B OH to facilitate the catalytic activity. The optimal catalyst exhibits a state-of-the-art turnover frequency (TOF) of 43 min −1 with considerable stability in NH 3 BH 3 hydrolysis. The rapid hydrogen generation during NH 3 BH 3 hydrolysis is ascribed to the integration of the active sites of B OH and CoP. Both experiments and theory demonstrate that reactant molecules (NH 3 BH 3 and H 2 O) adsorption and dissociation are mediated by the existence of B OH and CoP dual-active sites (B OH activates H 2 O, Co-P activates NH 3 BH 3 ). This work sheds fresh light on the design of efficient non-noble catalysts and motivates the exploration of hydrogen energy utilization technologies. CoP nanosheet supported on h-BN with surface-bonded water (CoP/h-BN OH ) is designed through a P-inducing strategy to stimulate the catalytic activity toward hydrogen generation. The catalyst exhibits a superior kinetics with favorable stability in hydrogen generation from ammonia borane hydrolysis. • CoP supported on h-BN with surface-bonded water was designed via a P-inducing strategy. • A TOF of 43 min −1 was achieved for NH 3 BH 3 hydrolysis on dual-active sites. • DFT calculation revealed the catalytic mechanism of B OH and CoP in hydrolysis reaction.","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"379 1","pages":"125729-125729"},"PeriodicalIF":0.0,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147331561","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zhimo Fang, Yuan Liang, Zepeng Zeng, Haotian Bai, Zhou Zhou, Lin Zhang, Bin Hu, Yang ShiGuan, Jihong Li, Qiang Lü
{"title":"Synergistic doping and defect engineering of CoS2 building electron cycle sites Co−N−Fe···SV for enhanced Fenton-like reaction","authors":"Zhimo Fang, Yuan Liang, Zepeng Zeng, Haotian Bai, Zhou Zhou, Lin Zhang, Bin Hu, Yang ShiGuan, Jihong Li, Qiang Lü","doi":"10.1016/j.apcatb.2025.125719","DOIUrl":"https://doi.org/10.1016/j.apcatb.2025.125719","url":null,"abstract":"","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"379 1","pages":"125719-125719"},"PeriodicalIF":0.0,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147330589","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zhexi Gao, Qian Wang, Haoran Ma, Huifang Wu, Richard Lewis, Dave Willock, Ouardia Akdim, Junting Feng, Graham J. Hutchings
{"title":"Asymmetrically coordinated Ru-O site facilitates H2 heterolytic cleavage for efficient green reductive amination of octanol to octylamine: A mechanistic investigation","authors":"Zhexi Gao, Qian Wang, Haoran Ma, Huifang Wu, Richard Lewis, Dave Willock, Ouardia Akdim, Junting Feng, Graham J. Hutchings","doi":"10.1016/j.apcatb.2025.125708","DOIUrl":"https://doi.org/10.1016/j.apcatb.2025.125708","url":null,"abstract":"The catalytic reductive amination of octanol exhibits a promising and environmentally friendly pathway for the synthesis of octylamine, a compound with significant applications in the bulk and fine chemical sectors. However, the complexity of this reaction lies in the necessity of a catalyst that can simultaneously facilitate both the dehydrogenation and hydrogenation steps, occurring during the reaction. Herein, we have addressed this issue by designing a Ru@TiOx/Mg9Al6Ti6Ox catalyst with Ru-Ru and Ru-O asymmetric coordination structure that leads to 100 % octanol conversion, 94.6 % octylamine selectivity and a turn over frequency of 73.41 h−1, while maintaining the same activity for 4 consecutive cycles. Those performances, firmly positioning our catalyst among the most advanced and efficient catalysts reported to date. Using EXAFS, in situ FTIR, kinetic isotope experiments, and DFT calculations, we proposed a mechanism where Ru-O coordination structure promote the heterolytic cleavage of H2, producing highly active H+/H- species that can achieve efficient hydrogenation without hindering the dehydrogenation process. This work not only provides a promising catalyst for industrial application, but presents a valuable catalyst design strategy that involves complex tandem dehydrogenation/hydrogenation reactions.","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"379 1","pages":"125708-125708"},"PeriodicalIF":0.0,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147333642","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Dual-metal-catalyzed Fenton-like reaction on CdxZn1-xS @biochar: Mechanistic insights into sulfide-metal interactions for water purification","authors":"Xiaohong Zhao, Jianhua Tong, Sai Bai, Jin Qian","doi":"10.1016/j.apcatb.2025.125654","DOIUrl":"https://doi.org/10.1016/j.apcatb.2025.125654","url":null,"abstract":"","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"379 1","pages":"125654-125654"},"PeriodicalIF":0.0,"publicationDate":"2025-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147332620","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}