Angewandte Chemie International Edition最新文献

筛选
英文 中文
Microdroplet-Driven Synthesis of a Metal-Organic Framework Catalyst. 微滴驱动金属-有机骨架催化剂的合成。
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-09-27 DOI: 10.1002/anie.202515006
Xiaowei Song,Juldeh Jallow,Chanbasha Basheer,Rashed S Bakdash,Abdullah Alaliwi,Abdulaziz A Alzamil,Richard N Zare
{"title":"Microdroplet-Driven Synthesis of a Metal-Organic Framework Catalyst.","authors":"Xiaowei Song,Juldeh Jallow,Chanbasha Basheer,Rashed S Bakdash,Abdullah Alaliwi,Abdulaziz A Alzamil,Richard N Zare","doi":"10.1002/anie.202515006","DOIUrl":"https://doi.org/10.1002/anie.202515006","url":null,"abstract":"We report a room-temperature synthesis of copper-based metal-organic frameworks (Cu-MOFs) using microdroplet chemistry, offering a fast and energy-efficient alternative to conventional solvothermal methods that typically require high temperatures, extended reaction times, and suffer from inhomogeneous mixing. The unique microdroplet environment significantly accelerates reaction kinetics, enabling the formation of uniform octahedral crystals within 1 h at ambient conditions. Comprehensive characterization by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier-transform infrared spectroscopy (FTIR), high-resolution mass spectrometry (HRMS), Brunauer-Emmett-Teller (BET) surface area analysis, and thermogravimetric analysis (TGA) confirmed the high crystallinity, thermal stability, and porous structure of the Cu-MOFs. Compared to conventionally prepared Cu-MOFs, those synthesized via microdroplet chemistry exhibit comparable surface areas with improved exposure of active sites. As a demonstration of their catalytic potential, the MOFs were employed in a microbubble-assisted air-water interface system for nitrogen fixation under ambient conditions. The system effectively converted atmospheric nitrogen into nitrate, showcasing the practical utility of these materials in green chemical transformations. This study shows that microdroplet and microbubble technologies are powerful and sustainable platforms for MOF synthesis and catalytic applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"88 1","pages":"e202515006"},"PeriodicalIF":16.6,"publicationDate":"2025-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153567","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
Cleavable Antibody‐Conjugated Aβ Specific Immune Exosome for Combination Alzheimer's Disease Immunotherapy 可切割抗体偶联的Aβ特异性免疫外泌体用于联合阿尔茨海默病免疫治疗
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-09-27 DOI: 10.1002/anie.202517917
Mengmeng Ma, Jing Wang, Wenbin Zhong, Zhenhua Li, Yanli Zhao
{"title":"Cleavable Antibody‐Conjugated Aβ Specific Immune Exosome for Combination Alzheimer's Disease Immunotherapy","authors":"Mengmeng Ma, Jing Wang, Wenbin Zhong, Zhenhua Li, Yanli Zhao","doi":"10.1002/anie.202517917","DOIUrl":"https://doi.org/10.1002/anie.202517917","url":null,"abstract":"Recent progress in antibody‐based immunotherapies for Alzheimer's disease (AD) brings a sense of cautious optimism after years of setbacks. However, these approaches remain constrained by suboptimal pharmacodynamics, modest clinical benefits, and pro‐inflammatory adverse effects. Here, we develop a β‐secretase‐responsive immunotherapeutic agent (ATExo‐cL‐aA) that synergistically targets amyloid‐β (Aβ) and neuroinflammatory response, achieving heightened efficacy while reducing the side effects associated with conventional antibody therapies. After intranasal administration, ATExo‐cL‐aA actively migrates to AD brains. Upon cleavage by overexpressed β‐secretase, ATExo‐cL‐aA releases aducanumab antibody (aA) and exosomes derived from Aβ antigen‐specific Tregs (ATExo), which jointly manage Aβ and inflammatory microglia, thereby synergistically eradicating Aβ and reducing pro‐inflammatory responses. In AD mouse models, ATExo‐cL‐aA demonstrates efficient brain accumulation, robust Aβ removal, microglial normalization, neuroinflammation attenuation, and synaptic preservation, ultimately leading to improved cognitive function. These findings highlight ATExo‐cL‐aA as next‐generation immunotherapeutics that transcend the limitations of conventional antibody‐based treatments for AD.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"92 1","pages":"e202517917"},"PeriodicalIF":16.6,"publicationDate":"2025-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153764","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
Organic Polymer Semiconductor Photocatalysts: From Building Block Design to Controllable Assembly. 有机聚合物半导体光催化剂:从积木设计到可控组装。
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-09-27 DOI: 10.1002/anie.202516199
Yan Zhuang,Han Li,Shuo Wang,Haowei Huang,Xianzhi Fu,Jinlin Long
{"title":"Organic Polymer Semiconductor Photocatalysts: From Building Block Design to Controllable Assembly.","authors":"Yan Zhuang,Han Li,Shuo Wang,Haowei Huang,Xianzhi Fu,Jinlin Long","doi":"10.1002/anie.202516199","DOIUrl":"https://doi.org/10.1002/anie.202516199","url":null,"abstract":"Organic polymer semiconductors are emerging as a promising class of photocatalysts because their highly tunable molecular structures and flexible morphological control offer unique advantages for overcoming the efficiency bottlenecks of traditional inorganic materials. However, the development of organic polymer photocatalysts largely relies on empirical, trial-and-error approaches. The understanding of their structure-activity relationship is insufficient, which significantly hinders the rational design and performance prediction of polymer photocatalysts. This review systematically outlines the structure-driven design strategies for polymer photocatalysts by focusing on two interconnected levels: molecular building block design and controllable assembly. Starting with the molecular building block design, strategies including monomer unit selection, functional group modification, and heteroatom doping are analyzed in detail for tuning the material's intrinsic electronic and photophysical properties. At the assembly level, we explore how strategies like morphological control, surface modification, and pore engineering can guide the controlled organization of polymers to optimize the final semiconductor architecture. By establishing the relationship between structure and properties at different scales, we aim to build a systematic structure-activity relationship for polymer photocatalysts, ultimately seeking to shift from empirical screening to rational design.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"18 1","pages":"e202516199"},"PeriodicalIF":16.6,"publicationDate":"2025-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153569","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
Defects Induced in Situ Reconstruction of CdS with Oxygen-Tolerance Up to 23% in the Photocatalytic CO2 Reduction. 光催化CO2还原中耐氧高达23%的CdS原位重构缺陷。
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-09-27 DOI: 10.1002/anie.202514577
Xiaoyu Liang,Pengcheng Feng,Xinxin Zhang,Yan Liang,Min Ji,Mei Dong,Shengyang Tao,Xinkui Wang,Min Wang
{"title":"Defects Induced in Situ Reconstruction of CdS with Oxygen-Tolerance Up to 23% in the Photocatalytic CO2 Reduction.","authors":"Xiaoyu Liang,Pengcheng Feng,Xinxin Zhang,Yan Liang,Min Ji,Mei Dong,Shengyang Tao,Xinkui Wang,Min Wang","doi":"10.1002/anie.202514577","DOIUrl":"https://doi.org/10.1002/anie.202514577","url":null,"abstract":"Direct driving the photocatalytic reduction of CO2 from air or flue gas to produce value-added chemicals and fuels is very challenging due to the suppressing effect of the more favorable thermodynamically oxygen reduction reaction (ORR). Herein, we presented a novel oxygen-involved reconstruction pathway on a unique defective CdS-D in the photocatalytic reduction of CO2. The material is highly tolerant to O2 and generates 2766.7 µmol g-1 h-1 of CO under visible light irradiation in the presence of up to 23% content of O2. Intriguingly, instead of inhibiting the performance of CO2 reduction, the presence of oxygen positively promotes it, CO generation rate is up to 5124 µmol g-1 h-1 after multiple experimental cycles. The meticulously structural analysis reveals that the CdS-D with abundant defects tended to accumulate photogenerated holes, and S2- is oxidized to SO4 2- in the presence of oxygen to produce Cd2SO4(OH)2 as the active center for preferable CO2 adsorption and inhibit the O2 adsorption, which is the root cause for the high tolerance of oxygen in CO2 reduction (CO2RR). This work reveals a unique reconstruction process of sulfides photo corrosion, which provides a new idea for realizing the direct conversion of low-concentration CO2 by omitting expensive carbon capture or purification in industrial carbon resource utilization.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"101 1","pages":"e202514577"},"PeriodicalIF":16.6,"publicationDate":"2025-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153568","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
Photochemical Spin‐State Switching of an All‐Organic Molecular System with Visible Light 可见光下全有机分子体系的光化学自旋态开关
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-09-27 DOI: 10.1002/anie.202515144
Joël Schlecht, Thomas Lohmiller, Philipp Thielert, Clara Douglas, Malte Gather, Sabine Richert, Oliver Dumele
{"title":"Photochemical Spin‐State Switching of an All‐Organic Molecular System with Visible Light","authors":"Joël Schlecht, Thomas Lohmiller, Philipp Thielert, Clara Douglas, Malte Gather, Sabine Richert, Oliver Dumele","doi":"10.1002/anie.202515144","DOIUrl":"https://doi.org/10.1002/anie.202515144","url":null,"abstract":"Controlling the spin state of a molecule using the spatiotemporal properties of visible light is of interest for spintronic devices in information technology or (bio)medical applications. We, herein, report an all‐organic visible light‐induced photochromic system than can switch from a diamagnetic (singlet) to a paramagnetic (triplet) state. This is realized by precisely tuning orbital symmetry and internal molecular strain in a [5]helicene scaffold substituted with an indanedione π‐acceptor. Irradiation with visible light at cryogenic temperatures gives a kinetically meta‐stable paramagnetic diradical state with a solvent‐dependent ground‐state multiplicity (triplet or singlet), which can be thermally switched back to its initial diamagnetic state.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"196 1","pages":"e202515144"},"PeriodicalIF":16.6,"publicationDate":"2025-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153866","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
Engineering Localized Aromaticity in Amine‐Embedded Polycyclic Aromatic Hydrocarbons for Narrowband Fluorescence Emitter 窄波段荧光发射器中胺包埋多环芳烃的工程定域芳香性研究
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-09-27 DOI: 10.1002/anie.202518763
Yimin Wu, Shengqiu Zhai, Yayin Deng, Xingliang Wang, Zhengyang Bin, Jingsong You
{"title":"Engineering Localized Aromaticity in Amine‐Embedded Polycyclic Aromatic Hydrocarbons for Narrowband Fluorescence Emitter","authors":"Yimin Wu, Shengqiu Zhai, Yayin Deng, Xingliang Wang, Zhengyang Bin, Jingsong You","doi":"10.1002/anie.202518763","DOIUrl":"https://doi.org/10.1002/anie.202518763","url":null,"abstract":"The development of narrowband fluorescent emitters remains a long‐standing challenge in organic optoelectronics. Herein, we present an aromaticity engineering approach based on a perylene core to construct highly efficient narrowband fluorescent emitters. Replacement of one naphthalene unit with a carbazole moiety enhances the localization of aromaticity, while extension of the π–conjugation further attenuates the aromaticity of the remaining naphthalene ring. This dual modulation effectively suppresses emission shoulder bands, yielding spectrally pure fluorescence. Consequently, the centrosymmetric <jats:italic>c</jats:italic>‐NaDTCz and the axially symmetric <jats:italic>a</jats:italic>‐NaDTCz exhibit sharp emissions at 536 and 600 nm, with narrow full widths at half‐maximum (FWHM) of 17 and 30 nm, respectively. When applied in OLEDs, the <jats:italic>c</jats:italic>‐NaDTCz‐based device displays sharp yellow emission peaking at 548 nm with a high external quantum efficiency (EQE) of 26.1%, while <jats:italic>a</jats:italic>‐NaDTCz delivers narrowband red electroluminescence at 610 nm, achieving a record‐high EQE of 27.8% for conventional red fluorescent emitters.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"17 1","pages":"e202518763"},"PeriodicalIF":16.6,"publicationDate":"2025-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153869","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
Achieving Near‐Infrared Organic Room‐Temperature Phosphorescence for High‐Resolution Immune Response Monitoring and Bioimaging 实现近红外室温有机磷光,用于高分辨率免疫反应监测和生物成像
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-09-27 DOI: 10.1002/anie.202511784
Yeyun Zhao, Xianbin Ma, Shisheng Cui, Jiamin Qu, Yuqi Wen, Kai Zhang, Gengchen Li, Yongfeng Zhang, Xiaoyuan Huang, Baicheng Mei, Tao Wang, Peng Sun, Jianbing Shi, Bin Tong, Hai‐Yan Xie, Zitong Liu, Zhengxu Cai, Yuping Dong
{"title":"Achieving Near‐Infrared Organic Room‐Temperature Phosphorescence for High‐Resolution Immune Response Monitoring and Bioimaging","authors":"Yeyun Zhao, Xianbin Ma, Shisheng Cui, Jiamin Qu, Yuqi Wen, Kai Zhang, Gengchen Li, Yongfeng Zhang, Xiaoyuan Huang, Baicheng Mei, Tao Wang, Peng Sun, Jianbing Shi, Bin Tong, Hai‐Yan Xie, Zitong Liu, Zhengxu Cai, Yuping Dong","doi":"10.1002/anie.202511784","DOIUrl":"https://doi.org/10.1002/anie.202511784","url":null,"abstract":"Organic near‐infrared (NIR) room‐temperature phosphorescent (RTP) materials hold great potential for bioimaging due to their ability to eliminate background noise and tissue autofluorescence. Here, we synthesized octa‐ring fused RTP molecules (TPP‐BN and TPP‐BF) with B─N coordination bonds via a two‐step reaction, enabling NIR phosphorescent emission at 819 nm and a 28.6 ms lifetime. Using PMMA‐b‐PEG as host and surfactant to stabilize the RTP molecules, we fabricated PMMA‐b‐PEG based nanoparticles (PNPs) with five‐fold brighter afterglow than conventional F127‐based methods (FNPs). We further developed a granzyme B (GrB)‐responsive nanoprobe (Q‐BFNP) that achieves specific and quantitative detection. In vivo studies demonstrated their ability to monitor and distinguish tumor immune response with the signal‐to‐background ratio (SBR) as high as 216.4. This study provides a new method for constructing NIR organic RTP probes and advances applications of RTP materials in real‐time, high‐contrast bioimaging and tumor immune monitoring.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"10 1","pages":"e202511784"},"PeriodicalIF":16.6,"publicationDate":"2025-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153703","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
Plasma‐Electrocatalysis Cascade Synthesis of Deuterated Ammonia 等离子体电催化级联合成氘化氨
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-09-27 DOI: 10.1002/anie.202515856
Kaiwen Yang, Yanmei Huang, Runchao Qin, Qixing Wang, Shuhe Han, Bin Zhang, Yifu Yu
{"title":"Plasma‐Electrocatalysis Cascade Synthesis of Deuterated Ammonia","authors":"Kaiwen Yang, Yanmei Huang, Runchao Qin, Qixing Wang, Shuhe Han, Bin Zhang, Yifu Yu","doi":"10.1002/anie.202515856","DOIUrl":"https://doi.org/10.1002/anie.202515856","url":null,"abstract":"Deuterated ammonia (ND<jats:sub>3</jats:sub>) exhibits growing market demand in the fields of chemical analysis, pharmaceutical industry and semiconductor manufacturing. Currently, industrial production of ND<jats:sub>3</jats:sub> relies on harsh conditions and complex processes, leading to high production cost and security risk. Herein, we propose a sustainable relay strategy to produce ND<jats:sub>3</jats:sub> by using air and deuterium oxide (D<jats:sub>2</jats:sub>O) as raw materials, including plasma‐driven air‐to‐NO<jats:sub>x</jats:sub> conversion and electrocatalytic NO<jats:sub>x</jats:sub><jats:sup>–</jats:sup>‐to‐ND<jats:sub>3</jats:sub> conversion. The insufficient supply of reactive deuterium (*D) leads to sluggish kinetics of electrocatalytic deuterium reaction. The well‐designed F modified cobalt (F–Co) catalyst exhibits a remarkable yield of 0.75 mmol h<jats:sup>−1</jats:sup> cm<jats:sup>−2</jats:sup> and a Faradaic efficiency of 80.43% for ND<jats:sub>3</jats:sub> at 200 mA cm<jats:sup>−2</jats:sup>. The combined results of characterizations reveal that fluorine (F) atom can boost D<jats:sub>2</jats:sub>O dissociation and suppress competing deuterium evolution reaction, thereby providing abundant *D for deuteration reaction. Notably, a pilot‐scale demonstration system, consisting of non‐thermal plasma, flow electrolyzer, air stripping and ammonia absorber, is constructed to produce practicable ND<jats:sub>3</jats:sub> solution (2.8 wt%) with ∼21.45 mmol h<jats:sup>−1</jats:sup> ND<jats:sub>3</jats:sub> production capability by using air and D<jats:sub>2</jats:sub>O as sources.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"19 1","pages":"e202515856"},"PeriodicalIF":16.6,"publicationDate":"2025-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153867","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
Near-Infrared Conjugated Macrocyclic BODIPYs for Photothermal Cancer Therapy. 用于光热癌症治疗的近红外共轭大环体。
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-09-27 DOI: 10.1002/anie.202511125
Fei Cheng,Taotao Qiang,Mingli Li,Ruilong Li,Zhigao Wang,Tony D James
{"title":"Near-Infrared Conjugated Macrocyclic BODIPYs for Photothermal Cancer Therapy.","authors":"Fei Cheng,Taotao Qiang,Mingli Li,Ruilong Li,Zhigao Wang,Tony D James","doi":"10.1002/anie.202511125","DOIUrl":"https://doi.org/10.1002/anie.202511125","url":null,"abstract":"With this research we developed a cyclization strategy that effectively converts radiative transitions (RTs) to non-radiative transitions (NRTs) during the decay process of BODIPY-based photosensitizers. Compared to BODIPY monomers, cyclization leads to a significant decrease in the HOMO-LUMO energy gap and a significant increase in the HOMO energy. In particular, the absorption spectrum of 7a exhibits a significant redshift, with the maximum absorption wavelength reaching 794 nm. Photophysical characterization indicates that the macrocyclic BODIPY derivatives 7(a-d) exhibit a reduced RT process. While, the crystal structure and theoretical calculations suggest that the molecular ring distortion enhances the intersystem crossing (ISC) ability of the macrocyclic BODIPY derivatives 7(a-d). In addition 7a-NPs constructed using DSPE-mPEG2000 encapsulation exhibit excellent water solubility, stability, and photothermal conversion efficiency (44.6%). The photothermal therapeutic performance of 7a-NPs was evaluated through in vitro cell and in vivo mice experiments. The results indicated that 7a-NPs could be enriched at the tumor site and exhibited strong tumor ablation ability using near-infrared radiation. Our findings suggest that the regulation of the RT to NRT conversion using an alkali-induced cyclization reaction is a useful strategy for preparing efficient photo-thermal conversion materials based on BODIPY.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"65 1","pages":"e202511125"},"PeriodicalIF":16.6,"publicationDate":"2025-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153570","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
Electronic Modification at Atomic Scale: Design and Preparation of Diatomic Structures by Atomic Layer Deposition for Methanol Steam Reforming 原子尺度上的电子修饰:用原子层沉积法设计和制备甲醇蒸汽重整的双原子结构
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-09-27 DOI: 10.1002/anie.202514431
Jinqiu Guo, Leisheng Che, Yuyao Qin, Yaqi Hu, Xiaolin Tai, Jin Yuan, Li Jin, Yue Lin, Hongbo Zhang
{"title":"Electronic Modification at Atomic Scale: Design and Preparation of Diatomic Structures by Atomic Layer Deposition for Methanol Steam Reforming","authors":"Jinqiu Guo, Leisheng Che, Yuyao Qin, Yaqi Hu, Xiaolin Tai, Jin Yuan, Li Jin, Yue Lin, Hongbo Zhang","doi":"10.1002/anie.202514431","DOIUrl":"https://doi.org/10.1002/anie.202514431","url":null,"abstract":"The electronic effects of bimetallic components in catalysis remain poorly understood. Herein, atomically dispersed transition metal (TM) modified platinum (Pt)‐based bimetallic catalysts were designed and synthesized with the atomic layer deposition (ALD) method. Methanol steam reforming (MSR) was selected as a probe reaction to investigate the atomic‐level electronic effects of nickel (Ni) and iron (Fe) on Pt species. In situ/ex situ characterizations, isotope labeling, and DFT calculations reveal that different transition metals and ALD cycles tune the Pt electronic structure, significantly affecting catalytic activity. Notably, the 10cNi/Pt<jats:sub>1</jats:sub>/CeO<jats:sub>2</jats:sub> catalyst exhibits optimal electronic modification, achieving the highest MSR and water‐gas shift (WGS) conversions and the lowest activation energies. Additionally, kinetic isotope effect studies confirm that hydrogen formation proceeds via methanol dehydrogenation coupled with WGS. These findings provide new insights into electronic modifications at atomic scales within the bimetallic components, offering valuable guidance for the design and development of advanced catalytic systems.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"1 1","pages":"e202514431"},"PeriodicalIF":16.6,"publicationDate":"2025-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153865","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
0
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
相关产品
×
本文献相关产品
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信