COMMUNICATIONS CHEMISTRY 是 NATURE RESEARCH 的一本开放获取期刊，发表化学科学所有领域的高质量研究、评论和评论。该杂志发表的研究论文代表了重大进展，为专业研究领域带来了新的化学见解。我们还旨在为所有化学家的重要问题提供一个社区论坛，无论其子学科如何。

Communications Chemistry is an open-access journal published by NATURE RESEARCH, dedicated to high-quality research, reviews, and commentaries across all areas of chemical science. The research papers published in this journal represent significant advancements, providing new insights into the field of chemistry. We also aim to offer a community forum for all chemists to discuss important issues, regardless of their sub-discipline.

《Communications Chemistry》是NATURE RESEARCH旗下的一本开放获取期刊，致力于发表化学科学各个领域的高质量研究论文、评论和综述。该期刊所刊登的研究成果代表了重要的科学进展，为专业领域带来了新的化学见解。此外，我们还旨在为所有化学家提供一个讨论重要问题的社区论坛，无论其研究的子学科是什么。

Communications Chemistry

Abstract Polyethylene terephthalate (PET), the most abundantly produced polyester plastic, can be depolymerized by the Ideonella sakaiensis PETase enzyme. Based on multiple PETase crystal structures, the reaction has been proposed to proceed via a two-step serine hydrolase mechanism mediated by a serine-histidine-aspartate catalytic triad. To elucidate the multi-step PETase catalytic mechanism, we use transition path sampling and likelihood maximization to identify optimal reaction coordinates for the PETase enzyme. We predict that deacylation is likely rate-limiting, and the reaction coordinates for both steps include elements describing nucleophilic attack, ester bond cleavage, and the “moving-histidine” mechanism. We find that the flexibility of Trp185 promotes the reaction, providing an explanation for decreased activity observed in mutations that restrict Trp185 motion. Overall, this study uses unbiased computational approaches to reveal the detailed reaction mechanism necessary for further engineering of an important class of enzymes for plastics bioconversion.

Tucker Burgin

Benjamin C. Pollard

Brandon C. Knott

Heather B. Mayes

Michael F. Crowley

John E. McGeehan

Gregg T. Beckham

H. Lee Woodcock

The reaction mechanism of the Ideonella sakaiensis PETase enzyme

Dynamic microscale droplets produced by liquid-liquid phase separation (LLPS) have emerged as appealing biomaterials due to their remarkable features. However, the instability of droplets limits the construction of population-level structures with collective behaviors. Here we first provide a brief background of droplets in the context of materials properties. Subsequently, we discuss current strategies for stabilizing droplets including physical separation and chemical modulation. We also discuss the recent development of LLPS droplets for various applications such as synthetic cells and biomedical materials. Finally, we give insights on how stabilized droplets can self-assemble into higher-order structures displaying coordinated functions to fully exploit their potentials in bottom-up synthetic biology and biomedical applications.

Mehwish Naz

Lin Zhang

Chong Chen

Shuo Yang

Hongjing Dou

Stephen Mann

Jianwei Li

Self-assembly of stabilized droplets from liquid–liquid phase separation for higher-order structures and functions

Abstract The sorbicillinoid family is a large class of natural products known for their structural variety and strong, diverse biological activities. A special member of this family, sorbicillactone A, the first nitrogen-containing sorbicillinoid, exhibits potent anti-leukemic and anti-HIV activities and possesses a unique structure formed from sorbicillinol, alanine, and fumaric acid building blocks. To facilitate in-depth biological and structure-activity relationship studies of this promising natural product, we developed a chemoenzymatic approach that provides access to sorbicillactone A and several analogs with excellent yields under precise stereochemical control. The key steps of the highly convergent, stereoselective, and short route are the enantioselective oxidative dearomatization of sorbillin to sorbicillinol catalyzed by the enzyme SorbC and the subsequent Michael addition of a fumarylazlactone building block. Additionally, our synthetic findings and bioinformatic analysis suggest that sorbicillactone A is biosynthetically formed analogously.

Jonas I Müller

Tobias A M Gulder

Chemoenzymatic total synthesis of sorbicillactone A

Abstract Corannulene (C 20 H 10 ) is a polycyclic hydrocarbon in which five six-membered rings surround a central five-membered ring to construct a bowl-like aromatic structure. Here we examine the development of synthetic strategies that allow for the growth of the peripheral aromatic rings as a means to extend the aromatic area of the central corannulene nucleus and provide access to unique nanocarbon molecules.

Ezzah M. Muzammil

Dzeneta Halilovic

Mihaiela C. Stuparu

Synthesis of corannulene-based nanographenes

Abstract Asparaginyl ligases have been extensively utilized as valuable tools for site-specific bioconjugation or surface-modification. However, the application is hindered by the laborious and poorly reproducible preparation processes, unstable activity and ambiguous substrate requirements. To address these limitations, this study employed a structure-based rational approach to obtain a high-yield and high-activity protein ligase called OaAEP1-C247A-aa55-351. It was observed that OaAEP1-C247A-aa55-351 exhibits appreciable catalytic activities across a wide pH range, and the addition of the Fe 3+ metal ion effectively enhances the catalytic power. Importantly, this study provides insight into the recognition and nucleophile peptide profiles of OaAEP1-C247A-aa55-351. The ligase demonstrates a higher recognition ability for the “Asn-Ala-Leu” motif and an N-terminus “Arg-Leu” as nucleophiles, which significantly increases the reaction yield. Consequently, the catalytic activity of OaAEP1-C247A-aa55-351 with highly efficient recognition and nucleophile motif, “Asn-Ala-Leu” and “Arg-Leu” under the buffer containing Fe 3+ is 70-fold and 2-fold higher than previously reported OaAEP1-C247A and the most efficient butelase-1, respectively. Thus, the designed OaAEP1-C247A-aa55-351, with its highly efficient recognition and alternative nucleophile options, holds promising potential for applications in protein engineering, chemo-enzymatic modification, and the development of drugs.

Jiabao Tang

Mengling Hao

Junxian Liu

Yaling Chen

Gulimire Wufuer

Jie Zhu

Xuejie Zhang

Tingquan Zheng

Mujin Fang

Shiyin Zhang

Tingdong Li

Shengxiang Ge

Jun Zhang

Ningshao Xia

Design of a recombinant asparaginyl ligase for site-specific modification using efficient recognition and nucleophile motifs

重组天冬酰胺基连接酶的设计用于高效识别和亲核基序的位点特异性修饰

Expanded phthalocyanines are a promising class of materials for optoelectronic applications, owing to their unique properties and versatile metal coordination reactivity. The expansion of their π-electron systems and resulting red-shifted absorption are of particular interest for achieving broader applications. Here, we report the on-surface synthesis of metallo-phthalocyanines with extended electron systems and an open-chain polycyanine from ortho-dicarbonitrile precursors on Ag(111) and Au(111), studied by scanning tunneling microscopy (STM) and X-ray photoelectron spectroscopy (XPS). The larger 6,7-di(2-naphthyl)-2,3-naphthalenedicarbonitrile (NND) undergoes spontaneous cyclotetramerization on the Ag(111) surface forming the corresponding silver naphthalocyanines (Ag-NPc), contrasting previous reports where a partially aliphatic ortho-dicarbonitrile precursor formed polycyanine chains. In contrast, monolayers of the smaller 6,7-diphenyl-2,3-naphthalenedicarbonitrile (PND) form the corresponding naphthalocyanine only in the presence of co-adsorbed iron atoms (Fe-NPc). In the absence of iron, PND multilayers form polycyanine chains and Ag-NPc. NND and PND further differ in their reactivity due to the supramolecular behavior of their products. While the larger Ag-NPc aggregates to non-covalent one-dimensional ribbons, the smaller Fe-NPc forms an extended non-covalent two-dimensional network. Our study demonstrates the versatility of on-surface dinitrile tetramerization for the synthesis of π-extended cyclic phthalocyanines and their open-chain polycyanine counterparts.

Lukas J. Heuplick

Qitang Fan

Dmitriy A. Astvatsaturov

Tatiana V. Dubinina

J. Michael Gottfried

On-surface synthesis of phthalocyanines with extended π-electron systems

表面合成具有扩展π电子体系的酞菁化合物

Communications Chemistry is pleased to introduce a Collection of research works focused on recent developments within the interdisciplinary field of on-surface synthesis. Here, the Guest Editors highlight key themes and look towards the future of this research field.

Jennifer MacLeod

Alexander Saywell

Ping Yu

Commun Chem

On-surface synthesis

表面合成研究

Non-metallic catalysis has been known as a remarkable development strategy for hydrofunctionalization of unsaturated hydrocarbons. Herein, we report a unique chemically active method of BF3·OEt2 promoted multi-component, highly regioselective, and chemoselective hydrothio(seleo)phosphonylation of unsaturated hydrocarbons, which exhibits high yield and good substrate universality. The reaction mechanism was further elucidated to be Markovnikov addition by controlling experiments, 31P and 19F NMR spectra tracking experiments, X-ray diffraction analysis, and DFT calculations. Furthermore, the gram-scale attempt and the application of the reaction on the derivatization of natural products have been successfully conducted, leading to the discovery of 3as with potential anti-Parkinson's disease (PD) activities at 1 μM. This streamlined and efficient methodology has established a new platform for non-metallic Lewis acids-promoted hydrofunctionalization of unsaturated hydrocarbons and its application on new drug research. Transition metal catalysts are typically used for the hydrofunctionalization of unsaturated hydrocarbons, however, such reactions are time-consuming and may be challenging. Herein, the authors report the non-metallic BF3·OEt2-promoted multi-component, highly regioselective, and chemoselective hydrothio(seleo)phosphonylation of unsaturated hydrocarbons, which exhibits high yields and good substrate universality

Chang-Wei Shao

Pei-Feng Wan

Quan Xu

Ze-Nan Yang

Mei-Yu Geng

Yu Zhang

Xing-Hua Zhang

Xu-Wen Li

Phosphinothio(seleno)ation of alkynes/olefins and application on the late-stage functionalization of natural products

炔烃/烯烃的膦硫（硒）化反应及其在天然产物后期功能化中的应用

Lipid-protein interactions are crucial for virtually all biological processes in living cells. However, existing structural databases focusing on these interactions are limited to integral membrane proteins. A systematic understanding of diverse lipid-protein interactions also encompassing lipid-anchored, peripheral membrane and soluble lipid binding proteins remains to be elucidated. To address this gap and facilitate the research of universal lipid-protein assemblies, we developed BioDolphin - a curated database with over 127,000 lipid-protein interactions. BioDolphin provides comprehensive annotations, including protein functions, protein families, lipid classifications, lipid-protein binding affinities, membrane association type, and atomic structures. Accessible via a publicly available web server ( www.biodolphin.chemistry.gatech.edu ), users can efficiently search for lipid-protein interactions using a wide range of options and download datasets of interest. Additionally, BioDolphin features interactive 3D visualization of each lipid-protein complex, facilitating the exploration of structure-function relationships. BioDolphin also includes detailed information on atomic-level intermolecular interactions between lipids and proteins that enable large scale analysis of both paired complexes and larger assemblies. As an open-source resource, BioDolphin enables global analysis of lipid-protein interactions and supports data-driven approaches for developing predictive machine learning algorithms for lipid-protein binding affinity and structures. Lipid–protein interactions are crucial for virtually all biological processes in living cells, however, systematic structural databases covering broad types of lipid–protein interaction are lacking. Here, the authors develop BioDolphin, a curated database with over 127,000 lipid–protein interactions, providing comprehensive annotations detailing lipid–protein complexes.

Li-Yen Yang

Kaike Ping

Yunan Luo

Andrew C. McShan

BioDolphin as a comprehensive database of lipid–protein binding interactions

BioDolphin：脂质-蛋白质结合相互作用的综合数据库

Abstract The potential energy landscape (PEL) formalism is a powerful tool within statistical mechanics to study the thermodynamic properties of classical low-temperature liquids and glasses. Recently, the PEL formalism has been extended to liquids/glasses that obey quantum mechanics, but applications have been limited to atomistic model liquids. In this work, we extend the PEL formalism to liquid/glassy water using path-integral molecular dynamics (PIMD) simulations, where nuclear quantum effects (NQE) are included. Our PIMD simulations, based on the q-TIP4P/F water model, show that the PEL of quantum water is both Gaussian and anharmonic. Importantly, the ring-polymers associated to the O/H atoms in the PIMD simulations, collapse at the local minima of the PEL (inherent structures, IS) for both liquid and glassy states. This allows us to calculate, analytically, the IS vibrational density of states (IS-VDOS) of the ring-polymer system using the IS-VDOS of classical water (obtained from classical MD simulations). The role of NQE on the structural properties of liquid/glassy water at various pressures are discussed in detail. Overall, our results demonstrate that the PEL formalism can effectively describe the behavior of molecular liquids at low temperatures and in the glass states, regardless of whether the liquid/glass obeys classical or quantum mechanics.

短名	Commun Chem
Journal Impact	5.96
国际分区	CHEMISTRY, MULTIDISCIPLINARY(Q1)
期刊索引	SCI Q2中科院 2 区

ISSN	2399-3669
h-index	44
国内分区	化学(2区)化学化学综合(2区)

涉及主题	化学有机化学物理生物材料科学生物化学量子力学工程类催化作用化学工程纳米技术物理化学冶金遗传学复合材料核磁共振计算机科学医学
出版信息	出版商: Springer Nature，出版周期: ，期刊类型: journal，开源期刊: 是
基本数据	创刊年份: 2018，原创研究文献占比: 95.21%，自引率:0.00%， Gold OA占比: 99.82%
期刊费用	$3690详情
平均审稿周期	网友分享经验：13 Weeks

Communications Chemistry

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