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Field-enhanced CO electroreduction in membrane electrolyzers at a dehydrated interface 脱水界面膜电解槽中的场增强型一氧化碳电还原
IF 23.5 1区 化学
Chem Pub Date : 2024-11-18 DOI: 10.1016/j.chempr.2024.10.019
Wenhao Ren, Huanlei Zhang, Miyeon Chang, Nanjun Chen, Wenchao Ma, Jun Gu, Meng Lin, Xile Hu
{"title":"Field-enhanced CO electroreduction in membrane electrolyzers at a dehydrated interface","authors":"Wenhao Ren, Huanlei Zhang, Miyeon Chang, Nanjun Chen, Wenchao Ma, Jun Gu, Meng Lin, Xile Hu","doi":"10.1016/j.chempr.2024.10.019","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.10.019","url":null,"abstract":"Zero-gap membrane electrode assembly (MEA) CO electrolyzer stands as a promising technology for circular carbon economy. However, current CO electrolyzers are energetically inefficient when operating at ampere-level current densities. Here, by analyzing the performance discrepancies between MEA and flow cells, we identify the depletion of K<sup>+</sup> and water at the cathode as the main contributor to the low performance of MEA CO electrolyzers. This is attributed to the unique cathodic interface in catholyte-free MEA, where there is no aqueous electrolyte to maintain the three-phase interface. Through the development of needle-array catalysts with intensified electric fields (EFs) at their tips, we are able to concentrate the limited K<sup>+</sup> cations onto the tips of the cathode, while simultaneously facilitating water uptake via electro-osmosis. We construct an MEA CO electrolyzer that achieves a large current density of 2,500 mA cm<sup>−2</sup> at a voltage of only 2.7 V.","PeriodicalId":268,"journal":{"name":"Chem","volume":"36 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665346","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}
引用次数: 0
Lighting up industrial mechanochemistry: Real-time in situ monitoring of reactive extrusion using energy-dispersive X-ray diffraction 点亮工业机械化学：利用能量色散 X 射线衍射对反应挤压进行实时原位监测
IF 19.1 1区 化学
Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.07.033
Nikita Y. Gugin , Kirill V. Yusenko , Andrew King , Klas Meyer , Dominik Al-Sabbagh , Jose A. Villajos , Franziska Emmerling
{"title":"Lighting up industrial mechanochemistry: Real-time in situ monitoring of reactive extrusion using energy-dispersive X-ray diffraction","authors":"Nikita Y. Gugin ,&nbsp;Kirill V. Yusenko ,&nbsp;Andrew King ,&nbsp;Klas Meyer ,&nbsp;Dominik Al-Sabbagh ,&nbsp;Jose A. Villajos ,&nbsp;Franziska Emmerling","doi":"10.1016/j.chempr.2024.07.033","DOIUrl":"10.1016/j.chempr.2024.07.033","url":null,"abstract":"<div><div>Mechanochemistry is an environmentally friendly synthetic approach that enables the sustainable production of a wide range of chemicals while reducing or eliminating the need for solvents. Reactive extrusion aims to move mechanochemistry from its conventional gram-scale batch reactions, typically performed in laboratory ball mills, to a continuous, large-scale process. Meeting this challenge requires <em>in situ</em> monitoring techniques to gain insights into reactive extrusion and its underlying processes. While the effectiveness of <em>in situ</em> Raman spectroscopy in providing molecular-level information has been demonstrated, our study uses energy-dispersive X-ray diffraction to monitor reactive extrusion in real time at the crystalline level. Our results provide previously unavailable control over the reactive extrusion process, promoting its perception as an industrially feasible green alternative to traditional solvent-based syntheses.</div></div><div><h3>Video abstract</h3><div><span><span><span><span><video><source></source></video></span><span><span>Download: <span>Download video (18MB)</span></span></span></span></span></span></div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3459-3473"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142085779","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}
引用次数: 0
Illuminating aromatic deuteration 照亮芳香族氘化
IF 19.1 1区 化学
Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.09.022
Da Zhao , Tobias Ritter
{"title":"Illuminating aromatic deuteration","authors":"Da Zhao ,&nbsp;Tobias Ritter","doi":"10.1016/j.chempr.2024.09.022","DOIUrl":"10.1016/j.chempr.2024.09.022","url":null,"abstract":"<div><div>Late-stage deuteration is a crucial technique in the pharmaceutical industry. Direct aromatic deuteration without the use of directing groups or transition-metal catalysts presents a substantial challenge. Now, through the integration of an interrupted Birch reduction, Liang, Xia, and co-workers have developed a photochemical protocol for the efficient hydrogen isotope exchange to incorporate deuterium into the arenes of pharmaceuticals.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3266-3267"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142487534","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}
引用次数: 0
Accurate triplet energies prediction method based on the hot-band model 基于热带模型的精确三重能预测方法
IF 19.1 1区 化学
Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.10.014
Wenbin Huang , Zhe Dong
{"title":"Accurate triplet energies prediction method based on the hot-band model","authors":"Wenbin Huang ,&nbsp;Zhe Dong","doi":"10.1016/j.chempr.2024.10.014","DOIUrl":"10.1016/j.chempr.2024.10.014","url":null,"abstract":"<div><div>In this issue of <em>Chem</em>, Popescu and Paton report a new method to predict triplet energy sensitization of small molecules by sampling the instantaneous vertical energy gaps over molecular vibrational motions. This approach has reduced the mean absolute error of predicting E<sub>T</sub> from 9.5 to 1.7 kcal/mol compared with previous state-of-the-art methods.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3270-3272"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142556260","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}
引用次数: 0
Atom swap in triple bonds via nitrogen-deletion coupling with gem-diborylalkanes 通过二硼烷的缺氮耦合实现三键中的原子交换
IF 19.1 1区 化学
Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.08.001
Liangxuan Xu , Du Chen , Peng Zhang , Chungu Xia , Chao Liu
{"title":"Atom swap in triple bonds via nitrogen-deletion coupling with gem-diborylalkanes","authors":"Liangxuan Xu ,&nbsp;Du Chen ,&nbsp;Peng Zhang ,&nbsp;Chungu Xia ,&nbsp;Chao Liu","doi":"10.1016/j.chempr.2024.08.001","DOIUrl":"10.1016/j.chempr.2024.08.001","url":null,"abstract":"<div><div>Alkynes have played pivotal roles in numerous synthetic transformations and materials science. Here, by developing nitrogen-deletion coupling, we describe a modular synthesis of alkynes from widely accessible nitriles by swapping the N atom to a C atom in cyano groups, where lithiated <em>gem</em>-diborylalkanes and <em>tert</em>-butyl nitrite are applied sequentially. NMR analysis and crystal structure show the nature of an intermediary α-boryl lithium enamine. A diverse range of nitriles are converted into various internal and terminal alkynes within a short reaction time, including alkynes bearing bulky secondary and tertiary alkyl substituents on both sides.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3474-3487"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142138192","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}
引用次数: 0
Steric-confinement Rh2/MoS2 dual-atom catalyst directionally modulating adsorption configuration of ester group to boost ethanol synthesis 立体构型 Rh2/MoS2 双原子催化剂定向调节酯基吸附构型，促进乙醇合成
IF 19.1 1区 化学
Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.06.015
Yi Zhao , Qingqing Gu , Xue Sun , Dong Wang , Xueqing Gong , Bing Yang , Jing Xu , Bo Peng , Ying Zhang , Chengsi Pan , Yongfa Zhu , Yang Lou
{"title":"Steric-confinement Rh2/MoS2 dual-atom catalyst directionally modulating adsorption configuration of ester group to boost ethanol synthesis","authors":"Yi Zhao ,&nbsp;Qingqing Gu ,&nbsp;Xue Sun ,&nbsp;Dong Wang ,&nbsp;Xueqing Gong ,&nbsp;Bing Yang ,&nbsp;Jing Xu ,&nbsp;Bo Peng ,&nbsp;Ying Zhang ,&nbsp;Chengsi Pan ,&nbsp;Yongfa Zhu ,&nbsp;Yang Lou","doi":"10.1016/j.chempr.2024.06.015","DOIUrl":"10.1016/j.chempr.2024.06.015","url":null,"abstract":"<div><div><span><span>Developing a new tactic for directionally regulating a specific functional group of feedstock molecules at the molecular level is highly desired to synthesize high-value products but remains challenging. We design and construct the two-dimensional </span>molybdenum disulfide (2D MoS</span><sub>2</sub><span>) nanosheets edge-anchored dual Rh atoms (Rh</span><sub>2</sub>/MoS<sub>2</sub><span> dual-atom catalyst [DAC]) to boost the ethanol yield in dimethyl oxalate (DMO) selective hydrogenation by precisely manipulating the DMO adsorption configuration. Comprehensive experimental and theoretical results reveal that the pocket-like active center of Rh</span><sub>2</sub><span> atoms, with a precise metal-metal distance (3.5 Å), realizes the spatially matched bidentate DMO adsorption via two C=O groups (distance of 3.1 Å), which remarkably enhances the DMO activation and drives the production of ethanol via a unilateral activation mechanism. The turnover frequency (TOF) and H</span><sub>2</sub>/DMO molar ratio of Rh<sub>2</sub>/MoS<sub>2</sub> DAC are around 19 times higher and 17 times lower, respectively, than those of the best reported catalysts under comparable conditions. Our results offer practical opportunities for updating the industrial syngas-DMO-ethanol route.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3342-3363"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141578005","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}
引用次数: 0
Atomically thin Ag nanosheets for single-molecule SERS detection of BPF 用于单分子 SERS 检测 BPF 的原子级薄银纳米片
IF 19.1 1区 化学
Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.06.020
Pengfei Hu , Haosen Yang , Rutong Si , Bin Wei , Xiaotian Wang , Ziyan Xu , Xiuyi Yang , Tianqi Guo , Ralph Gebauer , Gilberto Teobaldi , Li-Min Liu , Zhongchang Wang , Lin Guo
{"title":"Atomically thin Ag nanosheets for single-molecule SERS detection of BPF","authors":"Pengfei Hu ,&nbsp;Haosen Yang ,&nbsp;Rutong Si ,&nbsp;Bin Wei ,&nbsp;Xiaotian Wang ,&nbsp;Ziyan Xu ,&nbsp;Xiuyi Yang ,&nbsp;Tianqi Guo ,&nbsp;Ralph Gebauer ,&nbsp;Gilberto Teobaldi ,&nbsp;Li-Min Liu ,&nbsp;Zhongchang Wang ,&nbsp;Lin Guo","doi":"10.1016/j.chempr.2024.06.020","DOIUrl":"10.1016/j.chempr.2024.06.020","url":null,"abstract":"<div><div><span>Despite the exceptional properties and advanced functionalities of two-dimensional (2D) nanomaterials<span><span>, the fabrication of freestanding, atomically thin metal nanosheets poses a considerable challenge due to the inherently omnidirectional nature of typical </span>metallic bonds<span><span>. Herein, we introduce a novel ligand-confinement strategy to prepare the atomically thin Ag nanosheets. The ultrathin 2D structure is stabilized by manipulating the coordinate ligands to construct confined spaces and lower the inherent high surface energy, thus avoiding agglomeration. The atomically thin 2D structure exhibits a distinct quantum confinement effect, inducing </span>energy level splitting<span><span> conducive to uniform hot spots on planar Ag surfaces and extraordinary surface-enhanced Raman spectroscopy (SERS) properties. Leveraging the synergistic effects of </span>electromagnetic and chemical enhancement, our approach achieves single-molecule-level SERS detection at concentrations as low as 10</span></span></span></span><sup>−17</sup><span> M of bisphenol F (BPF). The atomically thin noble metal-based SERS technology possesses superb merits of ultra-high sensitivity, extraordinary uniformity, and reproducibility.</span></div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3364-3373"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141578128","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}
引用次数: 0
Oscillatory adaptive catalysis: Intramolecular chain shuttling regulated by stereo-autocorrection in stereoselective polymerization of lactide 振荡自适应催化：立体选择性聚合内酯过程中由立体自校正调节的分子链内穿梭
IF 19.1 1区 化学
Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.06.031
Wuchao Zhao , Fengchao Cui , Jianghua He , Yuetao Zhang , Eugene Y.-X. Chen
{"title":"Oscillatory adaptive catalysis: Intramolecular chain shuttling regulated by stereo-autocorrection in stereoselective polymerization of lactide","authors":"Wuchao Zhao ,&nbsp;Fengchao Cui ,&nbsp;Jianghua He ,&nbsp;Yuetao Zhang ,&nbsp;Eugene Y.-X. Chen","doi":"10.1016/j.chempr.2024.06.031","DOIUrl":"10.1016/j.chempr.2024.06.031","url":null,"abstract":"<div><div><span>In metal-mediated stereoselective polymerization of cyclic esters, racemic catalysts use their enantiomers for enantioselective roles and achieve diverse polymer stereomicrostructures through intermolecular chain exchange. Here, an intramolecular chain shuttling mechanism is achieved by the combination of </span><em>cis</em> (<em>R,S</em>)-dithiourea and MeOK to overcome limitations on intermolecular polymer exchange and also offer diverse polymer stereomicrostructures. This system exhibits diastereospecificity toward the polymerization of both <em>rac</em>-lactide (<em>rac</em>-LA) and <em>meso</em>-LA, producing highly isotactic PLA (<em>P</em><sub>m</sub> ∼ 0.96) and heterotactic PLA (<em>P</em><sub>r</sub><span><span> ∼ 0.92), respectively. Mechanistic studies reveal an “oscillatory adaptive catalysis” (OAC) phenomenon, which is key to achieving dual recognition of the </span>chirality<span> of both the chain end and incoming monomer<span> by using the two switchable chiral centers in catalyst. Such OAC enables dynamic interchange between chiral recognition (that triggers chain propagation) and stereochemical autocorrection (when monomer mismatched) by multi-site cooperativity, which induces chiral-site switching and polymer-chain shuttling intramolecularly within a single catalyst molecule.</span></span></span></div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3396-3409"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141746612","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}
引用次数: 0
Selective hydrogenation catalysis enabled by nanoscale galvanic reactions 利用纳米级电化反应实现选择性氢化催化
IF 19.1 1区 化学
Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.06.030
Mengfei Qiao , Qingyuan Wu , Ying Wang , Shanshan Gao , Ruixuan Qin , Shengjie Liu , Kehong Ding , Dongyuan Zhao , Nanfeng Zheng
{"title":"Selective hydrogenation catalysis enabled by nanoscale galvanic reactions","authors":"Mengfei Qiao ,&nbsp;Qingyuan Wu ,&nbsp;Ying Wang ,&nbsp;Shanshan Gao ,&nbsp;Ruixuan Qin ,&nbsp;Shengjie Liu ,&nbsp;Kehong Ding ,&nbsp;Dongyuan Zhao ,&nbsp;Nanfeng Zheng","doi":"10.1016/j.chempr.2024.06.030","DOIUrl":"10.1016/j.chempr.2024.06.030","url":null,"abstract":"<div><div><span>By mimicking nanoscale galvanic reactions, this study focuses on optimizing catalytic hydrogenation by introducing two spatially separated sites for the activation of H</span><sub>2</sub> into proton and electron pairs and the selective reduction of –NO<sub>2</sub>. The catalyst system is designed with the co-deposition of Pt and Fe<sub>2</sub>O<sub>3</sub><span><span> nanoparticles on conductive </span>carbon nanotubes<span>, establishing an electron-transferring pathway. Protic solvents facilitate proton transport. Upon activation of H</span></span><sub>2</sub> molecules into proton and electron pairs on Pt, modified with ammonia or amines, these active species are efficiently transferred to Fe<sub>2</sub>O<sub>3</sub><span> nanoparticles for the selective reduction of –NO</span><sub>2</sub> into amines without affecting other functional groups. Compared with Pt/CNT, which easily hydrogenates both C=C and –NO<sub>2</sub> groups of 4-nitrostyrene, the Pt&amp;Fe<sub>2</sub>O<sub>3</sub>/CNT catalyst modified by NH<sub>3</sub> exhibits higher activity and selectivity for –NO<sub>2</sub><span> hydrogenation. Electrochemically, Pt functions as the anode for the hydrogen oxidation reaction, while Fe</span><sub>2</sub>O<sub>3</sub> acts as the cathode, selectively reducing –NO<sub>2</sub>.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3385-3395"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141754488","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}
引用次数: 0
In situ energy dispersive X-ray diffraction achieved in twin screw extrusion 在双螺杆挤压中实现原位能量色散 X 射线衍射
IF 19.1 1区 化学
Chem Pub Date : 2024-11-14 DOI: 10.1016/j.chempr.2024.10.011
Edward J. Broker Jr. , Kathleen Floyd , James D. Batteas
{"title":"In situ energy dispersive X-ray diffraction achieved in twin screw extrusion","authors":"Edward J. Broker Jr. ,&nbsp;Kathleen Floyd ,&nbsp;James D. Batteas","doi":"10.1016/j.chempr.2024.10.011","DOIUrl":"10.1016/j.chempr.2024.10.011","url":null,"abstract":"<div><div>In the current issue of <em>Chem</em>, Gugin et al. are showcasing the power of energy-dispersive X-ray diffraction to track kinetics and chemical phenomena <em>in situ</em> during twin screw extrusion. This technique holds great promise for industrial scale-up of green chemical syntheses.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3268-3270"},"PeriodicalIF":19.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142562008","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}
引用次数: 0
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