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Disentangling the activity-selectivity trade-off in CO2 hydrogenation to methanol 解解CO2加氢制甲醇的活性-选择性权衡
IF 19.1 1区 化学
Chem Pub Date : 2026-08-13 Epub Date: 2026-03-13 DOI: 10.1016/j.chempr.2026.102942
Habib Zada, Jiafeng Yu (俞佳枫), Chuanyan Fang (方传艳), Jian Sun (孙剑)
{"title":"Disentangling the activity-selectivity trade-off in CO2 hydrogenation to methanol","authors":"Habib Zada,&nbsp;Jiafeng Yu (俞佳枫),&nbsp;Chuanyan Fang (方传艳),&nbsp;Jian Sun (孙剑)","doi":"10.1016/j.chempr.2026.102942","DOIUrl":"10.1016/j.chempr.2026.102942","url":null,"abstract":"<div><div>Cu-based catalysts for CO<sub>2</sub> hydrogenation show outstanding performance but often face an activity-selectivity trade-off. Herein, we introduced Cu nanoparticles onto ZnZr oxides via a sputtering method, inducing ZnO migration over Cu surfaces by a strong metal-support interaction. This enhances the CO<sub>2</sub> conversion by 5-fold compared with ZnZr oxide catalysts and achieves 92% methanol selectivity, significantly outperforming commercial CuZnAl (11%) at 300°C, resulting in a methanol space-time yield of 1.2 g⸱g<sub>cat</sub><sup>−1</sup>⸱h<sup>−1</sup>. Characterization reveals that the coverage suppresses CO<sub>2</sub> activation at Cu sites and C‒O bond breaking before hydrogenation to reduce CO production. CO<sub>2</sub> preferentially adsorbs on ZrO<sub>2</sub> sites with both O atoms, following a formate pathway, where activated H from Cu sites attacks C without breaking the O–C–O bonds. Decoupling activation sites drives the hydrogenation pathway toward methanol over CO, even at high temperatures. This spatial arrangement of catalytic sites provides key insights for designing high-performance catalysts by weakening undesired functions.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 8","pages":"Article 102942"},"PeriodicalIF":19.1,"publicationDate":"2026-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148718848","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
Chem at 10: Gabriela S. Schlau-Cohen 化学10:Gabriela S. Schlau-Cohen
IF 19.1 1区 化学
Chem Pub Date : 2026-08-13 DOI: 10.1016/j.chempr.2026.103157
Gabriela S. Schlau-Cohen
{"title":"Chem at 10: Gabriela S. Schlau-Cohen","authors":"Gabriela S. Schlau-Cohen","doi":"10.1016/j.chempr.2026.103157","DOIUrl":"10.1016/j.chempr.2026.103157","url":null,"abstract":"<div><div>Gabriela S. Schlau-Cohen, PhD, the Haslam-Dewey Professor of Chemistry at the Massachusetts Institute of Technology, was selected to participate in <em>Chem</em>’s 10<sup>th</sup> anniversary interview series because of her contributions to the journal in spectroscopy and photosynthetic light harvesting. In this Q&amp;A, she discusses the teachers who inspired her, the importance of carving one’s own path, and the excitement of making unexpected discoveries.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 8","pages":"Article 103157"},"PeriodicalIF":19.1,"publicationDate":"2026-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148718852","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
Skeletal editing by iron-catalyzed carbene insertion of trichloromethanes 由铁催化的三氯甲烷插入碳的骨骼编辑
IF 19.1 1区 化学
Chem Pub Date : 2026-08-13 Epub Date: 2026-03-26 DOI: 10.1016/j.chempr.2026.102968
Bethany M. DeMuynck, Ethan E. Hyland, Hojin Kim, Victoria L. Menches, Anna M.M. Vernier, Zhang Wang, David E. Olson, Mark D. Levin, David A. Nagib
{"title":"Skeletal editing by iron-catalyzed carbene insertion of trichloromethanes","authors":"Bethany M. DeMuynck,&nbsp;Ethan E. Hyland,&nbsp;Hojin Kim,&nbsp;Victoria L. Menches,&nbsp;Anna M.M. Vernier,&nbsp;Zhang Wang,&nbsp;David E. Olson,&nbsp;Mark D. Levin,&nbsp;David A. Nagib","doi":"10.1016/j.chempr.2026.102968","DOIUrl":"10.1016/j.chempr.2026.102968","url":null,"abstract":"<div><div>Direct interchange between five- and six-membered nitrogen heterocycles by skeletal editing is valuable in drug discovery. Specifically, inserting a carbon atom into oxidatively prone indole affords metabolically stable quinoline. However, tailored reagents for this transformation are limited by safety, availability, and generality. Here, we introduce a C-insertion method that employs stable, commercially abundant trichloromethanes (as chlorocarbene precursors) and simple iron catalysts (FeCl<sub>2</sub>) to directly transform indoles to diverse quinolines. This highly practical method allows rare access to direct C-H and C-D insertion (essential analogs in medicinal chemistry) and many other pharmacophores. Mechanistic studies show key differences in rate, reactivity, and selectivity of this iron carbene versus metal-free carbenes. In addition, the skeletal editing of several drug-like molecules is presented, including a one-step synthesis of a quinoline analog of the psychedelic indole lysergic acid diethylamide (LSD). This analog exhibits lower potency and efficacy for activating 5-HT2A receptors, suggesting therapeutic potential with reduced hallucinogenic properties.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 8","pages":"Article 102968"},"PeriodicalIF":19.1,"publicationDate":"2026-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147519117","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
High-entropy-inspired multi-principal single-atom materials 高熵激发多主单原子材料
IF 19.1 1区 化学
Chem Pub Date : 2026-08-13 Epub Date: 2026-07-23 DOI: 10.1016/j.chempr.2026.103153
Li Yu, Zhijun Wang, Zhengxiao Guo, Hao Ming Chen, Hsien-Yi Hsu
{"title":"High-entropy-inspired multi-principal single-atom materials","authors":"Li Yu,&nbsp;Zhijun Wang,&nbsp;Zhengxiao Guo,&nbsp;Hao Ming Chen,&nbsp;Hsien-Yi Hsu","doi":"10.1016/j.chempr.2026.103153","DOIUrl":"10.1016/j.chempr.2026.103153","url":null,"abstract":"<div><div>Emerging multi-principal single-atom materials (MPSAMs), including commonly known high-entropy single-atom materials, extend the design principles of high-entropy alloys into atomically dispersed frameworks. This perspective examines the developmental pathway of MPSAMs and describes how combining insights from high-entropy and related fields with the atomic precision of single-atom materials leads to unconventional reactivity patterns. We suggest that a range of observable features, from basic composition to specific structural and functional characteristics, can be used to inform entropy-inspired design of MPSAMs for nonlinear synergistic performance. Following the concept of chemical short-range order in alloy physics, a promising direction is to modulate the metal atom arrangement from completely random to partially correlated states, enabling tailored local ordering in MPSAMs. The advancement requires expanding synthetic protocols and developing multidisciplinary platforms that integrate complementary characterization, theoretical cross-validation, and automated workflows to achieve predictive catalyst screening and rational design.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 8","pages":"Article 103153"},"PeriodicalIF":19.1,"publicationDate":"2026-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148624226","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
Reaction: The art of autonomous chemistry 反应：自主化学的艺术
IF 19.1 1区 化学
Chem Pub Date : 2026-08-13 Epub Date: 2026-07-30 DOI: 10.1016/j.chempr.2026.103138
Florian Boser, Frank Glorius
{"title":"Reaction: The art of autonomous chemistry","authors":"Florian Boser,&nbsp;Frank Glorius","doi":"10.1016/j.chempr.2026.103138","DOIUrl":"10.1016/j.chempr.2026.103138","url":null,"abstract":"<div><div>Florian Boser holds an MSc in chemistry from LMU Munich. After a research stay with Prof. Lee Cronin in Glasgow, he joined Prof. Frank Glorius in Münster for his PhD on high-throughput experimentation, machine learning, and automation. Frank Glorius is a full professor of organic chemistry at the University of Münster. His interdisciplinary research focuses on new concepts for photocatalysis, asymmetric heterogeneous catalysis, arene hydrogenation, and organocatalysis. His group also studies functional molecules for surface modification, battery additives, or interfacing with biological membranes and develops data science and molecular machine-learning tools with practical relevance to synthetic chemistry.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 8","pages":"Article 103138"},"PeriodicalIF":19.1,"publicationDate":"2026-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148624233","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
Can polymer mechanochemistry stop a bullet? 高分子机械化学能阻挡子弹吗？
IF 19.1 1区 化学
Chem Pub Date : 2026-08-13 DOI: 10.1016/j.chempr.2026.103191
Sonja Storch, Robert Göstl
{"title":"Can polymer mechanochemistry stop a bullet?","authors":"Sonja Storch,&nbsp;Robert Göstl","doi":"10.1016/j.chempr.2026.103191","DOIUrl":"10.1016/j.chempr.2026.103191","url":null,"abstract":"<div><div>In the current issue of <em>Nature</em>, Johnson, Nelson, and coworkers demonstrate that mechanophore crosslinks can dramatically enhance ballistic impact resistance. By selectively releasing network constraints during extreme deformation, force-triggered chemistry enables local plastic flow in thermosets, revealing mechanochemistry as a design principle for materials operating far from equilibrium.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 8","pages":"Article 103191"},"PeriodicalIF":19.1,"publicationDate":"2026-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148718571","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
Stereoretentive radical-radical alkyl-alkyl cross-coupling by Ni-catalysis ni催化的立体保持自由基-自由基烷基-烷基交叉偶联
IF 19.1 1区 化学
Chem Pub Date : 2026-08-13 DOI: 10.1016/j.chempr.2026.103197
Qiong Yu, Wei Shu
{"title":"Stereoretentive radical-radical alkyl-alkyl cross-coupling by Ni-catalysis","authors":"Qiong Yu,&nbsp;Wei Shu","doi":"10.1016/j.chempr.2026.103197","DOIUrl":"10.1016/j.chempr.2026.103197","url":null,"abstract":"<div><div>Stereogenic C(sp<sup>3</sup>)–C(sp<sup>3</sup>) bond formation through catalytic radical-radical cross-coupling (RRCC) reactions relies heavily on stereoconvergent coupling of two alkyl precursors facilitated by chiral ligands or auxiliaries. In <em>Science</em>, Baran and coworkers developed a stereoretentive RRCC that directly couples two distinct transient alkyl radicals, derived from enantioenriched sulfonylhydrazides and achiral alkyl halides, in the presence of an achiral ligand, which enables the coupling of two alkyl radicals together with precise stereochemical control.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 8","pages":"Article 103197"},"PeriodicalIF":19.1,"publicationDate":"2026-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148718572","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
Design and organocatalytic enantioselective assembly of axially chiral boracyclohexylidenes and chiral boraspiranes 轴向手性硼环己基醚和手性硼aspiranes的设计和有机催化对映选择性组装
IF 19.1 1区 化学
Chem Pub Date : 2026-08-13 DOI: 10.1016/j.chempr.2026.103106
Shuai Wang, Jianbo Liu, Wangyang Li, Ying Li, Yanying Huang, Wenyue Ma, Qiuling Song
{"title":"Design and organocatalytic enantioselective assembly of axially chiral boracyclohexylidenes and chiral boraspiranes","authors":"Shuai Wang,&nbsp;Jianbo Liu,&nbsp;Wangyang Li,&nbsp;Ying Li,&nbsp;Yanying Huang,&nbsp;Wenyue Ma,&nbsp;Qiuling Song","doi":"10.1016/j.chempr.2026.103106","DOIUrl":"10.1016/j.chempr.2026.103106","url":null,"abstract":"","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 8","pages":"Article 103106"},"PeriodicalIF":19.1,"publicationDate":"2026-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148718575","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
Superlattice electrocatalysis matching microbial metabolism for sustainable CO2-to-bioproduct conversion 超晶格电催化与微生物代谢相匹配，实现二氧化碳到生物产品的可持续转化
IF 19.1 1区 化学
Chem Pub Date : 2026-08-13 Epub Date: 2026-03-19 DOI: 10.1016/j.chempr.2026.102955
Miao Liu, Yanfeng Shi, Hao Shi, Peilin Huang, Lupeng Wang, Zhujun Fu, Tianming Wu, Yuanhong Xu
{"title":"Superlattice electrocatalysis matching microbial metabolism for sustainable CO2-to-bioproduct conversion","authors":"Miao Liu,&nbsp;Yanfeng Shi,&nbsp;Hao Shi,&nbsp;Peilin Huang,&nbsp;Lupeng Wang,&nbsp;Zhujun Fu,&nbsp;Tianming Wu,&nbsp;Yuanhong Xu","doi":"10.1016/j.chempr.2026.102955","DOIUrl":"10.1016/j.chempr.2026.102955","url":null,"abstract":"<div><div>The integrated electrochemical-microbial system (iEMS) is a promising strategy for converting CO<sub>2</sub> into high-value bioproducts. However, the mismatch in the carbon species and flux between electrocatalysis and microbial metabolism hinders its overall efficiency. Herein, we develop a scalable Ag/Cu metal superlattice (MSL@Ag/Cu) electrocatalyst with a periodic electric-potential gradient, which enables the selective and stable production of microbe-biased ethanol substrate and maintains carbon flux for the iEMS. The directional Ag/Cu configuration causes a spatial confinement effect, which enriches and holds the key intermediates for sustainable C–C coupling. MSL@Ag/Cu achieves a high Faradaic efficiency of ethanol (&gt;61.1%) and maintains this efficiency for over 220 h at 200 mA cm<sup>−2</sup> in an industrial electrolyzer. This long-term ethanol yield (160 mmol L<sup>−1</sup>) with indispensable carbon flux of <em>Saccharomyces cerevisiae</em> enables the breakthrough conversion of CO<sub>2</sub> to bioproducts. Techno-economic analysis indicates that the iEMS generates a profit of $15.5 million per year, which is 15-fold that of traditional electrocatalytic synthesis.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 8","pages":"Article 102955"},"PeriodicalIF":19.1,"publicationDate":"2026-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147479072","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
Advances in polymer chemistry enabled by transition metal catalysis 过渡金属催化使聚合物化学取得进展
IF 19.1 1区 化学
Chem Pub Date : 2026-08-13 Epub Date: 2026-07-08 DOI: 10.1016/j.chempr.2026.103140
Christopher Rybak, Christopher Uyeda
{"title":"Advances in polymer chemistry enabled by transition metal catalysis","authors":"Christopher Rybak,&nbsp;Christopher Uyeda","doi":"10.1016/j.chempr.2026.103140","DOIUrl":"10.1016/j.chempr.2026.103140","url":null,"abstract":"<div><div>Since the discovery of titanium catalysts for the synthesis of isotactic polypropylene, transition metal catalysis has played a central role in providing access to high-performance polymers. In this perspective, we present case studies that highlight the different ways that catalytic reactions initially developed for small-molecule chemistry are being used to tackle some of the most urgent challenges in polymer chemistry. The discussion is divided into three parts: polymerization reactions, polymer functionalization reactions, and polymer backbone editing reactions. Many of these methods target the synthesis of functional materials that can be used in drug delivery systems, electronic devices, membrane separators, and renewable energy conversion and storage technologies. Another area of interest is the development of degradable polymers from renewable feedstocks with comparable material properties to polyethylene or polypropylene. In a complementary strategy for sustainability, catalytic reactions can be used to functionalize or depolymerize waste plastics in recycling and upcycling schemes.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 8","pages":"Article 103140"},"PeriodicalIF":19.1,"publicationDate":"2026-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148624222","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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