ChemCatChemPub Date : 2024-08-27DOI: 10.1002/cctc.202481601
Prof. Nao Tsunoji, Misae Onishi, Sou Sonoda, Dr. Takeshi Ohnishi, Prof. Masaru Ogura, Prof. Zen Maeno, Prof. Takashi Toyao, Prof. Ken-ichi Shimizu
{"title":"Front Cover: Synthesis-Structure-Catalysis Relations in CHA Zeolites Applied for Selective Catalytic Reduction of NOx with Ammonia (ChemCatChem 16/2024)","authors":"Prof. Nao Tsunoji, Misae Onishi, Sou Sonoda, Dr. Takeshi Ohnishi, Prof. Masaru Ogura, Prof. Zen Maeno, Prof. Takashi Toyao, Prof. Ken-ichi Shimizu","doi":"10.1002/cctc.202481601","DOIUrl":"https://doi.org/10.1002/cctc.202481601","url":null,"abstract":"<p><b>The Front Cover</b> represents the three formation routes of zeolite from different starting materials. Zeolites are crucial industrial catalysts, whereas their crystallization mechanism is still unclear, limiting their rational functional design. Nao Tsunoji and co-workers present the synthesis–structure–catalysis relation of CHA zeolite to get fundamental knowledge for intentionally controlling the function of zeolites. Different starting materials provide three different formation pathways to form CHA zeolites with different properties in the presence of tetraethylammonium hydroxide as an inexpensive organic structure directing agent. The knowledge related to origin of the catalytic durability was obtained based on their structural character, crystallization mechanism, and exhaust gas purification ability. More information can be found in the Research Article by Nao Tsunoji and co-workers (DOI: 10.1002/cctc.202400459).\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"16 16","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202481601","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142084581","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ChemCatChemPub Date : 2024-08-27DOI: 10.1002/cctc.202401271
Ms. Yilin Li, Dr. Xiaohan Gao, Dr. Xuechuan Iv, Dr. Ying Duan, Dr. Dong Sui, Wanting Chang, Dr. Yanliang Yang
{"title":"Recent Progress on Cobalt-Based Heterogeneous Catalysts for Hydrogen Production from Ammonia Borane","authors":"Ms. Yilin Li, Dr. Xiaohan Gao, Dr. Xuechuan Iv, Dr. Ying Duan, Dr. Dong Sui, Wanting Chang, Dr. Yanliang Yang","doi":"10.1002/cctc.202401271","DOIUrl":"10.1002/cctc.202401271","url":null,"abstract":"<p>Ammonia borane (NH<sub>3</sub>BH<sub>3</sub>, AB) is a quintessential exemplar of chemical hydrogen storage materials and has been widely used in hydrogen evolution. Although expensive metal catalysts (such as Rh, Ru, Pt, Ag, etc.) exhibit high activity in the hydrolysis of ammonia borane, inexpensive metals are more economical. Cobalt (Co), in particular, is not only relatively inexpensive and readily available, but also possesses high activity and selectivity. Compared to other catalysts, cobalt-based catalysts have better durability and can maintain catalytic activity for a longer period of time, making them favored by researchers. These catalysts demonstrate excellent stability, hydrogen evolution rate, and turn over frequency. This article summarized previous progress in low price metal cobalt-based catalysts for hydrogen precipitation from ammonia borane, focusing on cobalt-based catalysts supported on various supports, especially those supported on carbon materials, metal oxides, MOFs, and nickel foams. The characteristics of high-performance catalytic systems are analyzed in detail. The development prospects of Co catalysts for hydrogen production from ammonia borane were also discussed. In summary, this review compiles various supported and other types of cobalt based catalysts in recent years, and also identifies the existing problems with these catalysts, providing a reference for developers to study these catalysts. It is believed that through careful regulation of the electronic and spatial structures of Co based catalysts, well-designed Co based non precious metal catalysts will play a significant role in the decomposition of ammonia borane.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"16 23","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208789","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ChemCatChemPub Date : 2024-08-27DOI: 10.1002/cctc.202481602
Dr. Mengjiao Wang, Prof. Silvio Osella, Dr. Bruno Torre, Matteo Crisci, Fabian Schmitz, Roberto Altieri, Prof. Enzo Di Fabrizio, Dr. Heinz Amenitsch, Dr. Barbara Sartori, Zheming Liu, Prof. Teresa Gatti, Dr. Francesco Lamberti
{"title":"Cover Feature: Stabilizing Layered BiOBr Photoelectrocatalyst by Van Der Waals Heterojunction Strategy (ChemCatChem 16/2024)","authors":"Dr. Mengjiao Wang, Prof. Silvio Osella, Dr. Bruno Torre, Matteo Crisci, Fabian Schmitz, Roberto Altieri, Prof. Enzo Di Fabrizio, Dr. Heinz Amenitsch, Dr. Barbara Sartori, Zheming Liu, Prof. Teresa Gatti, Dr. Francesco Lamberti","doi":"10.1002/cctc.202481602","DOIUrl":"https://doi.org/10.1002/cctc.202481602","url":null,"abstract":"<p>2D MoS<sub>2</sub>/BiOBr van der Waals heterojunctions can be used for photoelectrocatalytic hydrogen production. <b>The Cover Feature</b> shows a MoS<sub>2</sub>/BiOBr heterojunction working as a photocathode. The photogenerated electrons from BiOBr mainly flow into two directions: one is migrating towards the MoS<sub>2</sub> surface, driving the hydrogen evolution reaction; the other is accumulating on BiOBr and reduces BiOBr to metallic Bi. However, in a heterojunction with small ratio of MoS<sub>2</sub>, the electrons are prone to transfer to MoS<sub>2</sub>, thus decreasing the accumulation of electrons on BiOBr and preventing it from deactivation. More information can be found in the Research Article by Mengjiao Wang, Francesco Lamberti, and co-workers (DOI: 10.1002/cctc.202400282).\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"16 16","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202481602","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142084582","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ChemCatChemPub Date : 2024-08-27DOI: 10.1002/cctc.202401421
Beikai Ding, Dr. Chengsheng Yang, Yue Chen, Wei-Peng Shao, Dr. Fan Yang, Chi Zhang, Dr. Zheng Wang, Prof. Dr. Yongmei Liu, Prof. Dr. Yong Cao, Prof. Dr. Yifeng Zhu, Dr. Xinhe Bao
{"title":"Cr2O3 Clusters on ZnO as Hydrogen Pools for Efficient Syngas-To-Light Olefins","authors":"Beikai Ding, Dr. Chengsheng Yang, Yue Chen, Wei-Peng Shao, Dr. Fan Yang, Chi Zhang, Dr. Zheng Wang, Prof. Dr. Yongmei Liu, Prof. Dr. Yong Cao, Prof. Dr. Yifeng Zhu, Dr. Xinhe Bao","doi":"10.1002/cctc.202401421","DOIUrl":"10.1002/cctc.202401421","url":null,"abstract":"<p>Interfaces of mixed oxide are often considered the primary catalytic sites, yet the functionalities of the surrounding environments are less understood. Composite oxides, particularly ZnO-Cr<sub>2</sub>O<sub>3</sub>, show high activity and selectivity for syngas conversion, with ZnO dissociating H<sub>2</sub> to hydrides and Cr<sub>2</sub>O<sub>3</sub> activating CO. However, hydrides on ZnO cannot remain stable at temperatures above room temperature. Focusing on the puzzlingly high performance despite ZnO's inability to stabilize active hydrides at reaction temperatures (300–400 °C), we clarified the roles of each phase using models of Cr<sub>2</sub>O<sub>3</sub>/ZnO and ZnO/Cr<sub>2</sub>O<sub>3</sub>. Cr<sub>2</sub>O<sub>3</sub> clusters on ZnO effectively stabilize and store hydrides, significantly enhancing syngas conversion compared to individual oxides or ZnO/Cr<sub>2</sub>O<sub>3</sub>. An acetate/ketene pathway on Cr<sub>2</sub>O<sub>3</sub>/ZnO was identified, driven by the unique role of Cr<sub>2</sub>O<sub>3</sub> clusters in regulating local hydride and CO coverages, unlike other routes observed on ZnO/Cr<sub>2</sub>O<sub>3</sub>. These insights advance the understanding of the active structures and functionalities of mixed oxides in catalysis.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"16 23","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208794","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ChemCatChemPub Date : 2024-08-27DOI: 10.1002/cctc.202401284
Bin Guan, Jiale Liu, Ji-dong Leng, Ting Fan, Lianpeng Tong
{"title":"Hydrogen Evolution Catalysis by Cobalt Complexes of an Aza-Bridged Bis-1,10-Phenanthroline Ligand Bearing Pendant Basic Sites","authors":"Bin Guan, Jiale Liu, Ji-dong Leng, Ting Fan, Lianpeng Tong","doi":"10.1002/cctc.202401284","DOIUrl":"10.1002/cctc.202401284","url":null,"abstract":"<p>A novel series of molecular Co(II) complexes with aza-bridged bis-1,10-phenanthroline (bpa) ligands have been synthesized and reported for the catalytic hydrogen evolution reaction (HER). Various nitrogen donor substituents are introduced at the aza-bridge of the bis-phenanthroline moieties render intramolecular basic sites in the complexes’ second-coordination sphere. Modifying the pendant nitrogen donor significantly influences the catalytic HER performance. Among these, the cobalt complex with the (2-pyridyl)methyl substituted bis-phenanthroline ligand (<b>L3</b>) exhibits the most photocatalytic HER efficiency in both organic and aqueous media. Under optimized conditions with [Ru(bpy)<sub>3</sub>]<sup>2+</sup> as a sensitizer and ascorbic acid as an electron donor, [Co<sup>II</sup>(<b>L3</b>)(TfO<sup>−</sup>)<sub>2</sub>] achieves an initial turnover frequency (TOF) of 1882±65 h<sup>−1</sup> per catalyst and a turnover number (TON) of 4842±122 in a 3 hour reaction period under the irradiation of visible light. Combined experimental and theoretical evidences illustrate that phenanthroline moieties of the bpa ligands act as electron mediators during the HER catalysis, while the pendant nitrogen donor substituents mediate proton transfer. This work provides a unique example for understanding the activity-structure relationship of homogeneous HER catalyst concerning the redox-active properties and second coordination sphere basic sites of organic ligand platforms.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"16 23","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208818","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ChemCatChemPub Date : 2024-08-26DOI: 10.1002/cctc.202400883
Simon Rydzek, Florian Guth, Steffen Friedrich, Jakob Noske, Birte Höcker, Frank Hahn
{"title":"Chemoenzymatic Synthesis of Plant-Derived Kavalactone Natural Products by Dynamic Resolution Using a Biosynthetic O-Methyltransferase Tailoring Enzyme","authors":"Simon Rydzek, Florian Guth, Steffen Friedrich, Jakob Noske, Birte Höcker, Frank Hahn","doi":"10.1002/cctc.202400883","DOIUrl":"10.1002/cctc.202400883","url":null,"abstract":"<p>Biosynthetic enzymes have enormous potential for the chemoenzymatic synthesis of natural products and other bioactive compounds. Methyltransferases are promising tools for the selective enzymatic modification of complex structures. This paper describes the production, purification and biochemical characterization of the O-methyltransferase JerF, which catalyzes unique 4-methoxy-5,6-dihydropyranone formation in jerangolid A biosynthesis. Isolation problems had hitherto prevented detailed studies on JerF and were solved by the fusion to maltose-binding protein. The differentiation of JerF between styryl-substituted dihydropyrandion enantiomers was investigated. In combination with a spontaneous racemization occurring with this type of substrates, a new enzymatic dynamic kinetic resolution was observed, which was used for the enantioselective chemoenzymatic synthesis of kavalactone natural products and new derivatives. In combination with an HMT-based SAM regeneration system, (+)-kavain, (+)-11,12-dimethoxykavain and (+)-12-fluorokavain were prepared in 3–4 steps on a 100 μmol scale with overall yields of 37–57 % and <i>ee</i>s of 70–86 %. A mutational study based on an AlphaFold 2 model provided indications for active site residues with an influence on the performance of the enzyme that could be targeted for engineering in the future. This example illustrates how the exceptional enzymatic activities and specificities of biosynthetic enzymes can be exploited for the development of new synthesis approaches.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"16 23","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202400883","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208821","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ChemCatChemPub Date : 2024-08-26DOI: 10.1002/cctc.202401255
Jiawen Hu, Suliang Wang, Lingna Wang, Dr. Jinguo Long, Prof. Dr. Xianjie Fang
{"title":"Tandem Hydrocyanation and Nitrile/Amide Cyclization of Propiolamides: A Rapid Access to 5-Iminopyrrolones","authors":"Jiawen Hu, Suliang Wang, Lingna Wang, Dr. Jinguo Long, Prof. Dr. Xianjie Fang","doi":"10.1002/cctc.202401255","DOIUrl":"10.1002/cctc.202401255","url":null,"abstract":"<p>A Pd-catalyzed synthesis of 5-iminopyrrolones from propiolamides was developed, which featured wide substrate scope and good yields. This efficient conversion involved a tandem hydrocyanation, <i>E</i> to <i>Z</i> isomerization of alkenes, and nitrile/amide cyclization. Control experiments show the intermediacy of <i>β</i>-cyanation products, and the Z-isomers was efficiently converted to the target products by Pd/<b>L2</b> catalysis only after the cyanation reagent was completely consumed.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"16 23","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208820","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Fabrication of FeCu/CC Composite for Efficient Removal of Nitrate for Aqueous Solution Via Electrochemical Reduction Process","authors":"Weiman Li, Qingbo Yin, Cuicui Liu, Shuqin Yang, Dongyu Jin, Xiuli Wang, Laizhou Song","doi":"10.1002/cctc.202401017","DOIUrl":"10.1002/cctc.202401017","url":null,"abstract":"<p>The electrochemical nitrate reduction (ENR) for the conversion of nitrate to nitrogen gas is a significant strategy to remediate the eutrophication in surface water. However, the exploitations and practical applications of suitable electrocatalysts still face great challenges. In this study, FeCu bimetal microparticles were deposited onto surface of carbon cloth (CC) to fabricate the FeCu/CC electrocatalyst for the removal of nitrate. Among obtained catalysts, the sample with Fe/Cu molar ratio of 1 : 15 (Fe<sub>1</sub>Cu<sub>15</sub>/CC) exhibits the excellent electroreduction efficiency for nitrate removal (R(NO<sub>3</sub><sup>−</sup>), >90 %) but an ineffective selectivity of N<sub>2</sub> formation (S(N<sub>2</sub>), ~23 %). After the anchor of reduced graphite oxide (rGO) to surface of Fe<sub>1</sub>Cu<sub>15</sub>/CC, at the optimized condition without the assistance of chlorine oxidation, R(NO<sub>3</sub><sup>−</sup>) and S(N<sub>2</sub>) of rGO/Fe<sub>1</sub>Cu<sub>15</sub>/CC catalyst reach 94.2 % and 72.8 %. After 5 day endurance test, the values of R(NO<sub>3</sub><sup>−</sup>) and S(N<sub>2</sub>) are still 82.9 % and 62.8 %, demonstrating the promising durability of this catalyst electrode. Meanwhile, the potential application of rGO/Fe<sub>1</sub>Cu<sub>15</sub>/CC was explored for the treatment of simulated wastewater discharged by urban wastewater treatment plant, the concentration of total nitrogen (TN) decreases from 15–1.17 mg/L, and this value is lower than TN threshold limit in Class IV of Chinese surface water quality standard.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"16 23","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-08-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208823","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ChemCatChemPub Date : 2024-08-23DOI: 10.1002/cctc.202401326
Mario Falsaperna, Rosa Arrigo, Frank Marken, Simon J. Freakley
{"title":"Alkali Metal Iridates as Oxygen Evolution Catalysts Via Thermal Transformation of Amorphous Iridium (oxy)hydroxides.","authors":"Mario Falsaperna, Rosa Arrigo, Frank Marken, Simon J. Freakley","doi":"10.1002/cctc.202401326","DOIUrl":"10.1002/cctc.202401326","url":null,"abstract":"<p>Efficient water-splitting is severely limited by the anodic oxygen evolution reaction (OER). Iridium oxides remain one of the only viable catalysts under acidic conditions due to their corrosion resistance. We have previously shown that heat-treating high-activity amorphous iridium oxyhydroxide in the presence of residual lithium carbonate leads to the formation of lithium-layered iridium oxide, suppressing the formation of low-activity crystalline rutile IrO<sub>2</sub>. We now report the synthesis of Na-IrO<sub>x</sub> and K-IrO<sub>x</sub> featuring similarly layered crystalline structures. Electrocatalytic tests confirm Li-IrO<sub>x</sub> retains similar electrocatalytic activity to commercial amorphous IrO<sub>2</sub> ⋅ 2H<sub>2</sub>O and with increasing size of the intercalated cation, the activity towards the OER decreases. However, the synthesised electrocatalysts that contain layers show greater stability than crystalline rutile IrO<sub>2</sub> and amorphous IrO<sub>2</sub> ⋅ 2H<sub>2</sub>O, suggesting these compounds could be viable alternatives for industrial PEM electrolysers where durability is a key performance measure.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"16 23","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202401326","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208827","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ChemCatChemPub Date : 2024-08-22DOI: 10.1002/cctc.202401202
Mohammad Misbahur Rahman, Dr. Indranil Dutta, Dr. Sandeep Suryabhan Gholap, Giao N. Ngô, Dr. Yadagiri Rachuri, Lujain Alrais, Prof. Kuo-Wei Huang
{"title":"Ruthenium Catalyzed Additive-Free N-Formylation of Amines with CO2 and H2: Exploring Carbon Neutral Hydrogen Cycle","authors":"Mohammad Misbahur Rahman, Dr. Indranil Dutta, Dr. Sandeep Suryabhan Gholap, Giao N. Ngô, Dr. Yadagiri Rachuri, Lujain Alrais, Prof. Kuo-Wei Huang","doi":"10.1002/cctc.202401202","DOIUrl":"https://doi.org/10.1002/cctc.202401202","url":null,"abstract":"<p>The <i>N</i>-formylation of amines using CO<sub>2</sub> hydrogenation, conducted under additive-free conditions, represents a crucial methodology in organic synthesis. Herein, we demonstrated a highly efficient ruthenium pincer complex for the selective conversion of a wide array of amines into their corresponding formamides under additive-free condition with a turnover number (TON) of 980,000 within a single-batch. Controlled studies suggested the initial reduction of CO<sub>2</sub> to ammonium formate, followed by dehydration to generate formamide. NMR experiments revealed the potential intermediates and indicated the involvement of metal-ligand cooperativity of catalyst during substrate activation. In addition, this methodology was examined to establish a carbon neutral hydrogen storage cycle by capitalizing on the reversible transformation of formamides.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"16 23","pages":""},"PeriodicalIF":3.8,"publicationDate":"2024-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142861974","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}