nature synthesis

Nature Synthesis

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Nature Synthesis aims to bring together researchers from all areas of chemical and materials synthesis, publishing work based on organic, inorganic, organometallic and materials chemistry as well as interdisciplinary studies at the interfaces between these disciplines.  The journal will be focused on the development of new synthetic methods and approaches, together with the preparation of molecular- or materials-based products that have practical value or that extend our conceptual understanding of chemical or material systems.

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Nature Synthesis

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Novel design strategy advances discovery of metal-organic frameworks

An innovative strategy, known as the "Up-Down Approach," has the potential to dramatically accelerate the creation of metal-organic frameworks (MOFs). The paper is published in the journal Nature Synthesis.

Analytical Chemistry

Sep 5, 2024

Chemists develop new sustainable reaction for creating unique molecular building blocks

Polymers can be thought of like trains: Just as a train is composed of multiple cars, polymers are made up of multiple monomers, and the couplings between the train cars are similar to the chemical bonds that link monomers ...

Aug 8, 2024

Building blocks for the future: Rhodium-catalyzed [2+2+1] cycloaddition achieves high enantioselectivity

Cycloaddition reactions are an efficient strategy for constructing cyclic compounds that are important building blocks for other chemicals. In these processes, π-electrons from different unsaturated molecules, such as alkenes, ...

Jul 26, 2024

Research team overcomes heteroatom constraints via cobalt catalysis

Professor Fu Yao and Associate Professor Lu Xi from the University of Science and Technology of China (USTC) have conducted a cobalt-hydride-catalyzed enantioselective hydroalkylation, enabling the efficient construction ...

Jul 24, 2024

'Janus' dual-atom catalyst shows enhanced performance for electrocatalytic oxygen reduction and evolution

A research team led by Prof. Yan Wensheng from the University of Science and Technology of China (USTC) has created the innovative "Janus" dual-atom catalyst (FeCo-N3O3@C) with Fe and Co atoms coordinated synergistically ...

Moving from the visible to the infrared: Developing high quality nanocrystals

Awarded the 2023 Nobel Prize in Chemistry, quantum dots have a wide variety of applications ranging from displays and LED lights to chemical reaction catalysis and bioimaging. These semiconductor nanocrystals are so small—on ...

Bio & Medicine

Jul 9, 2024

Rethinking old reaction mechanisms to obtain drug-type molecules

Nitrogen is an important and abundant element on Earth. In fact, nitrogen in the gas state is the most abundant gas in the atmosphere. This element is in our body as part of our DNA and in the center of hemoglobin. But nitrogen ...

Jul 1, 2024

New approach sets stage to explore the mirror-image world of century-old naturally-occurring cyclodextrins

Cyclodextrins (CDs), a class of cyclic oligosaccharides that were "born" in 1891, have opened up endless research and commercial opportunities in numerous fields that span carbohydrate, supramolecular (host-guest) and analytical ...

Biochemistry

Jun 24, 2024

Novel synthesis of fluorinated molecules with potential in drug research

Carboxylic acids are one of the most important substance classes in chemistry and are a component of many drugs such as aspirin and ibuprofen. To tailor the properties of carboxylic acids, fluorine atoms can be introduced ...

Jun 21, 2024

New photocatalytic COFs mimic photosynthesis for H₂O₂ production

National University of Singapore (NUS) chemists have developed hexavalent photocatalytic covalent organic frameworks (COFs) which mimic natural photosynthesis for the production of hydrogen peroxide (H2O2), an important industrial ...

Jun 14, 2024

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Nature cardiovascular research, nature synthesis and nature reviews psychology to launch under the nature portfolio imprint in 2022.

Two new transformative journals and a review journal provide a venue for cross-disciplinary research in the natural, applied and social sciences

London | New York | Berlin, 11 March 2021

Three new journals will be launched under the Nature Portfolio imprint at the beginning of 2022. These journals aim to meet the needs of different research communities by providing a venue for research not well served by existing publications. All three titles will be published online-only, and Nature Synthesis and Nature Cardiovascular Research will be Transformative Journals (Tjs), thereby enabling Plan S-funded authors, and others wishing to publish open access (OA), to submit primary research to these journals while  complying with their funders’ requirements. The journals will join the high-quality products and services of the Nature Portfolio, spanning the life, physical, chemical and applied sciences.

Like all Nature-branded journals, the new launches will be operated by a team of professional editors who oversee the careful selection, commissioning, fair and rigorous peer-review, accurate editing, rapid publication and broad dissemination of primary research and/or commissioned content.

Nature Cardiovascular Research is dedicated to publishing original and important advances in basic, translational, clinical and public health research focused on cardiac and vascular function and haematology in health and disease.

“Cardiovascular disease causes one-third of deaths worldwide and represents an urgent threat to global health*. Disease prevention as well as finding cure, treatment, and diagnostic tools depend upon advances in our understanding of the aetiology, molecular mechanisms and socioeconomic factors that drive and affect the disease. Nature Cardiovascular Research will provide a unifying publishing forum for all cardiovascular and haematology disciplines, ensuring that publications reach the widest possible audience of scientists, clinicians and policymakers,” explains Vesna Todorović, Chief Editor of Nature Cardiovascular Research .

Nature Synthesis aims to bring together researchers from both industry and academia from all areas of chemical and materials synthesis. Original research on organic, inorganic, organometallic and materials chemistry as well as technological innovations of value to the synthetic research community will be considered for publication. Nature Synthesis , which will be headed by Chief Editor Ali Stoddart, marks a move further into the applied sciences for the Nature Portfolio. 

Nature Reviews Psychology is the first Nature Reviews journal in the social and behavioral sciences. It will publish authoritative, accessible and topical Review, Perspective and Comment articles across the entire spectrum of psychological science, its applications and its wider societal implications. Jenn Richler is Chief Editor of Nature Reviews Psychology .

Ruth Wilson, Publishing Director Nature Journals, said: “Our new Nature Portfolio journals provide a wide range of research communities with publication venues for influential research aimed at a broad audience. As part of our wider commitment to open science, the two Transformative Journals, Nature Synthesis and Nature Cardiovascular Research , help improve the efficiency of the research process and strengthen the robustness of research output. Nature Reviews Psychology , as the first Nature Reviews journal in the social sciences, will publish timely, concise and accessible reviews for a new audience.” 

* Global burden of 369 diseases and injuries in 204 countries and territories, 1990–2019: a systematic analysis for the Global Burden of Disease Study 2019 . The Lancet . October 17, 2020.  

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Nature Synthesis

This journal aims to bring together researchers from all areas of chemical and materials synthesis, publishing work based on organic, inorganic, organometallic and materials chemistry as well as interdisciplinary studies at the interfaces between these disciplines.

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Harnessing nature's biosynthetic capacity to facilitate total synthesis

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Haili Zhang, Ge Liao, Xiaozhou Luo, Xiaoyu Tang, Harnessing nature's biosynthetic capacity to facilitate total synthesis, National Science Review , Volume 9, Issue 11, November 2022, nwac178, https://doi.org/10.1093/nsr/nwac178

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Natural products (NPs) have long piqued the interests of chemists due to their structural complexity. More importantly, evolution has conferred NPs with the ability to interact with biological macromolecules (such as nucleic acids, proteins, carbohydrates and lipids), making them privileged scaffolds for drug discovery. Until now, >50% of clinically approved drugs have been derived directly from NPs or their derivatives [ 1 ]. The difficulty in obtaining sufficient materials from their source organisms has been a major challenge in developing novel medicines from NPs. Although synthetic chemistry has arguably advanced to the point at which organic chemists can synthesize practically all NP types, producing most NPs through total synthesis within a reasonable cost and time range remains difficult.

Fundamentally, NPs are genetically encoded and biosynthesized. Over the last few decades, tremendous efforts have been made to elucidate NP biosynthesis, resulting in an expanding enzymatic repertoire available for the synthesis of NPs via synthetic biology. In this perspective, we use three representative examples to illuminate how synthetic biology is emerging in the field of total synthesis and highlight its prospects.

The first example is the bacteriostatic NP enterocin ( 8 ) from Streptomyces (Fig.  1 A). The unique tricyclic-caged skeleton of 8 has long fascinated biochemists and chemists, who have worked to solve its biosynthesis and pursue its chemical synthesis, respectively. Moore and colleagues figured out its biosynthetic procedure after over a decade of work [ 2–4 ]. Overall, enterocin biosynthesis begins with the assembly of a phenylalanine-derived benzoyl-CoA starter unit and seven malonyl-CoA through a multiprotein enzymatic complex called iterative type II polyketide synthase to produce a highly reactive intermediate 1 . During the chain elongation process, a reductase (EncD) selectively reduced the C7 keto group to yield the dihydrooctaketide ( 2 ). Oxidation of the C4 methylene group by the flavoprotein EncM triggers a Favorskii-like rearrangement and two intramolecular aldol condensations to form the caged tricyclic core (Fig. 1 A). Besides, enterocin was reconstructed in vitro by biosynthetic enzymes, indicating the first total enzymatic synthesis of a complex NP [ 3 ]. Knowledge of enterocin biosynthesis eventually inspired the development of the first chemical total synthesis of enterocin [ 5 ]. The essential step in the synthesis was designed to imitate the two aldol condensations involved in enterocin biosynthesis, resulting in the accomplishment of four of the seven stereogenic centers within the biomimetic reaction cascade (Fig. 1 A).

Our second example involves the first-line antimalarial drug, artemisinin ( 12 ), a sesquiterpene lactone containing an unusual peroxide bridge (Fig. 1 B). Since its discovery in the 1970s by Chinese scientists from Artemisia annua , artemisinin-based combination therapies have been the central drugs for treating malaria. However, the traditional avenue of obtaining artemisinin (isolated from A. annua ) depends on the weather and overall harvest, resulting in the shortage of supply and price fluctuations. Aiming to provide a stable source, Keasling and colleagues developed a microbial chemical factory by inserting a few artemisinin biosynthetic genes into Saccharomyces cerevisiae , to produce the late-stage artemisinin precursor artemisinic acid ( 9 ) at 100 mg/L [ 6 ]. Then, they employed several synthetic biology strategies, including promoter engineering, codon optimization and functional gene replacement, to enhance the yeast's ability to produce 9 , achieving improved titers of ≤25 g/L [ 7 ]. This accomplishment enabled them to establish a scalable synthetic route for easily converting artemisinic acid into artemisinin, with a singlet oxygen source serving as the critical step [ 8 ]. This study represents new ground in synergizing the abilities of synthetic biology and chemistry to solve intractable problems in the supply of naturally limited valuable chemicals.

Enzymes are often granted with strict substrate specificity; thus, developing total enzymatic synthesis of unnaturally complex molecules has been a daunting challenge. Ongoing advances in enzyme engineering, along with the ever-increasing enzymology knowledge, have now brought this stretched goal within reach. A terrific example involves a multi-enzymatic cascade for the synthesis of the nucleoside analog islatravir ( 16 ) [ 9 ], an alkyne- and fluorine-containing anti-HIV medication being investigated by Merck. The cascade was designed based on the reversibility of the bacterial nucleoside salvage pathway, which degrades purine 2 ′′ -deoxyribonucleosides in nature using a purine nucleoside phosphorylase (PNP), a phosphopentomutase (PPM) and a deoxyribose-5-phosphate aldolase (DERA) (Fig. 1 C). To accomplish this incredible task, the authors first engineered these enzymes to bear three non-natural substrates, including a fluorinated base, an alkyne-substituted ribose 5-phosphate and an aldehyde precursor. As the pathway favors digestion, the synthesis struggled significantly with low conversion. This problem was solved by introducing a sucrose phosphorylase to eliminate the inorganic phosphate by-product from the final reaction mixture, thereby promoting the reaction equilibrium towards 16 (Fig. 1 C). The authors further established a biosynthetic route for producing 2-ethynylglyceraldehyde-3-phosphate ( 15 ) for the DERA. Two engineered and immobilized enzymes (a galactose oxidase and pantothenate kinase) and three auxiliary enzymes catalyse the conversion, which starts from simple achiral building block 2-ethynylglycerol ( 13 ). Together, five engineered enzymes and four auxiliary enzymes were employed to stereoselectively assemble islatravir in three linear steps (51% overall yield). As the process eliminated intermediate purification and protection, the product was produced with fewer steps and a higher yield than the previously reported chemical synthesis (12 steps, 15% overall yield) [ 10 ]. This work is a tour de force that indicates a different approach in the synthesis of complex chemicals by harnessing the capacity of biosynthetic enzymes.

Applications of synthetic biology in total synthesis of complex molecules. (A) Enzymatic and chemical total synthesis of enterocin ( 8 ). (B) Fermentation and semi-synthesis of artemisinin ( 12 ). (C) Enzymatic synthesis of the deoxyadenosine analogue islatravir ( 16 ).

As evidenced above, we might be entering a new era in the total synthesis of small molecules with the emergence of synthetic biology. Overall, synthetic biology offers great efficiency, unbeatable precision and indispensable sustainability in chemical production, whereas chemical synthesis provides greater variability and diversity. Therefore, future advances in small molecule synthesis will be driven by a combination of chemistry and biology. Given the complexities of these two fields, it will be difficult for synthetic chemists or biologists to drive the amalgamation alone. We believe that a community effort is urgently needed to transform the field of total synthesis. In return, it will lay the foundation for improving our ability to control the shape and topology of complex small molecules.

X.T. acknowledges the support from the National Natural Science Foundation of China (82173719) and the Shenzhen Bay Laboratory Start-up Funds (21230051). X.L. acknowledges the support from the National Key Research and Development Program of China (2018YFA0903200) and the Shenzhen Institute of Synthetic Biology Scientific Research Program (JCHZ20200004).

Conflict of interest statement . X.L. has a financial interest in Demetrix.

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Introduction

近年来，随着蛋白质工程和生物信息学的飞速发展，功能性蛋白质的开发和应用变得越来越普遍。其中，蛋白酶作为天然的生物催化剂，具有着重要的研究价值和广阔的应用场景。作为合成化学和合成生物学的交叉领域，生物催化研究聚焦于挖掘新颖的酶催化过程，通过高效的酶促方法学解决传统的化学合成难题，同时实现生产成本的降低以及可持续性发展。与传统的小分子催化剂相比，蛋白质催化剂具有可基因编码和调控的特性，可以通过定向进化等手段进行高通量的筛选优化。

本课题关注的烯酮类化合物是合成化学中的重要中间体，可以参与多种经典的化学转化。同时，烯酮类结构在生物活性分子中广泛存在，比如蛋白的共价抑制剂等。大量的文献报道此类分子可作为黄素依赖酶OYE (old yellow enzyme) 的底物，发生经典的1,4-还原反应。然而，为了得到烯酮类化合物，传统的化学方法主要依赖于较强的氧化剂或者昂贵的过渡金属催化剂，发展高效的生物催化方法从而制备这类化合物十分必要。

2024年7月1日，北京生命科学研究所 / 清华大学生物医学交叉研究院刘臻实验室与西班牙赫罗纳大学Marc Garcia-Borràs团队合作，在 《Nature Synthesis》 杂志发表了题为  “Biocatalytic desymmetrization for synthesis of chiral enones using flavoenzymes”  的研究论文。 本研究分别利用黄素依赖酶的氧化和还原过程实现了立体手性互补的烯酮化合物的合成。 具体而言，本研究一方面发展了一种基于黄素依赖酶的不对称脱氢反应体系，通过酶催化的去饱和化过程，高对映选择性地 合成含季碳手性中心的环己烯酮类化合物 。通过分子动力学模拟以及DFT计算的手段，结合机理实验，作者深入地研究了这一酶催化的反应历程。基于对反应机理的探究，作者随后发现 如果利用还原态的黄素酶对环己二烯酮进行不对称还原，则可以获得相反构型的环己烯酮对映体产物 。这两种酶催化方法反应条件温和，操作简单，底物适用范围广泛，不管是催化脱氢还是不对称还原反应均可达到优异的底物转化率和高对映选择性。因此，这些方法有望在药物、天然产物等精细化学品的不对称合成中得到应用。

由于从环己酮类底物出发直接进行脱氢转化是合成烯酮类化合物最为简洁的合成方案之一，研究人员首先致力于通过 酶促不对称脱氢反应 来合成目标化合物。尽管自然界中存在不少类型的脱氢酶，然而真正被化学家关注且应用于合成中的例子屈指可数。本研究中，实验人员首先关注到文献记载了一种发现于嗜热菌株中的 GkOYE蛋白 具有一定的脱氢活性，尽管进一步调研发现相关文献并未成功展示这类酶在手性环己烯酮类化合物合成中的应用前景。

为了探究具有高热稳定性的黄素依赖酶是否可以作为优良的手性催化剂制备环己烯酮，研究人员以GkOYE作为参考序列，使用BLAST工具搜索具有序列相似性的蛋白，最终确定并成功表达了多个文献中尚未研究的热稳定性OYE。 后续的筛选实验表明，GkOYE和四种新发现的黄素酶均可以有效地催化底物1a的脱氢反应，并以良好的收率 (≥70%) 和优异的对映选择性 (99% e.e.) 得到目标产物2a。 其中，来源于Parageobacillus thermantarcticus中的黄素酶 (PtOYE) 表现出了最高的活性。值得一提的是，这一反应使用的唯一氧化剂为空气中的氧气， 因此比现有的化学催化方法更为清洁和温和 。

在确定了最优酶催化剂PtOYE和最适反应条件之后，研究人员系统地研究了这一酶促脱氢反应的底物适用范围。 实验结果表明，这种生物催化脱氢方法展示出了令人惊讶的底物兼容性和官能团耐受性。 具体而言，该方法可以兼容一系列不同电性的官能团，包括苯环上不同取代位置的吸电子或给电子基团，以及杂环，稠环和螺环等复杂结构。值得注意的是，氧化敏感性官能团如硫醚也可被该反应体系兼容，凸显了使用温和氧化剂进行脱氢反应的优势。另外，其他取代模式如4,4-双烷基或4-羟基-4-芳基取代的环己酮也同样适用于这一生物催化体系。 最后，研究人员意外发现 PtOYE-C26S单位点突变体可以显著提高酶催化效率 ，体现了这类脱氢酶仍然具有被进一步优化的潜力。

实验人员随后成功将这一酶催化反应放大至毫摩尔级乃至克级规模，并展示了烯酮类化合物的多种下游转化，制备了包括卤代环己烯酮、硅氧双烯和环氧环己酮在内的多种手性合成单元， 进一步证明了该酶催化方法的实用性和目标产物的合成价值 。

为了探究反应机理，作者通过计算与实验相结合的方式对这一酶促脱氢反应进行了研究。首先，工作人员利用分子动力学模拟 (MD simulations) 展示了底物与酶分子可能的结合模式。 通过计算模拟，作者发现活性空腔中的氨基酸残基H164可以通过与环己酮的羰基形成氢键，参与锚定底物；Y169残基在去质子后可作为关键的碱从环己酮底物的α位攫取质子，使其转化为水相中不稳定的烯醇中间体。 该中间体可以在一定程度上被活性口袋附近的极性氨基酸 (如H164、H167、K109和Y169) 所稳定，随后立体选择性的将β-氢转移至氧化态的FMN辅因子中，从而得到R-构型的环己烯酮产物。DFT能量计算进一步支持了这一机理的合理性。随后，研究人员通过定点突变实验验证了关键氨基酸残基的作用。 突变研究结果表明，对H164、H167、K109和Y169等四个氨基酸残基的突变显著降低了酶反应的转化效率。 此外，氢氘交换实验支持了Y169作为碱参与形成烯醇中间体的关键作用。

尽管研究人员已成功开发出一种高效的生物催化脱氢系统来获得高立体选择性的烯酮产物，但考虑到两种对映异构体在合成化学中的同等重要性，研究团队希望能够通过酶催化方法进一步获得相反构型的产物。 受酶促脱氢机理的启发，研究人员设想如果将环己酮底物替换成环己二烯酮化合物，两者与蛋白酶结合的模式应当相似。 由于烯烃还原反应将发生于之前环己酮底物脱氢的同一侧，因此目标产物中环己烯酮的双键位置将与脱氢过程得到的双键位置相反。令人高兴的是，作者的设想在后续的实验中得到了成功的验证。 经过对酶催化剂的筛选和反应条件的优化，作者发现YqjM酶可以高效地催化环己二烯酮化合物3a的不对称还原过程 (获得98%的产率和 >99%的e.e.)。随后的底物普适性研究进一步表明，这一酶促还原反应同样具有广泛的底物兼容性。

总的来说，利用互补的脱氢与还原转化为获得两种对映异构体的手性烯酮化合物提供了高效且立体选择性的合成方法，凸显了基于黄素依赖酶的去对称化策略在合成化学中的应用价值。 这项工作为合成含有手性季碳中心的环己烯酮提供了高效、绿色且立体可控的新策略，在有机合成和药物开发等领域具有重要的应用前景。

本项目的主要内容由刘臻实验室2022级PTN项目的研究生曾清清以及科研助理周谦一完成，其他作者包括2022级TIMBR项目研究生代双玉，科研助理赵翔以及西班牙赫罗纳大学的Carla Calvó-Tusell博士。刘臻研究员和Marc Garcia-Borràs研究员为本文的通讯作者。本研究得到科技部、清华大学生物医学交叉研究院以及北京生命科学研究所的资助。

https://www.nature.com/articles/s44160-024-00596-4

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Synthesis and Optical-Electronic Characterization of Nickel Pyro-Vanadate A 2 NiV 2 O 7 (A = Na, Ag) Semiconductors: Experimental, DFT, and Hybrid-DFT Approaches

• Brief Communication
• Published: 12 September 2024

Cite this article

• Atika Ayad 1 ,
• Elhassan Benhsina 2 ,
• Abdelqader El Guerraf   ORCID: orcid.org/0000-0002-5221-8656 3 &
• Souad El Hajjaji 1 , 4  

Semiconductors, with their exceptional properties, have diverse applications across fields such as photovoltaics, sensing, and catalysis. In the present study, nickel pyro-vanadate compounds of high purity and homogeneity, with the chemical formula A 2 NiV 2 O 7 (where A  = Na, Ag), were synthesized under precisely controlled stoichiometric conditions. The primary focus is to investigate the optical and electronic properties of these compounds using a combination of experimental techniques and theoretical modeling. Initially, insights into the chemical structure and morphology of the synthesized semiconductor were obtained through powder x-ray diffraction (PXRD), Fourier-transform infrared spectroscopy (FTIR), and scanning electron microscopy (SEM). A 2 NiV 2 O 7 were found to be homogeneous, crystalline in nature, and isotypic with Κ 2 CoV 2 O 7 , exhibiting alternating layers of NiV 2 O 7 and Ag/Na. Moreover, absorption spectra obtained from UV–Vis diffuse reflectance spectroscopy (DRS) showed direct optical bandgaps of 1.83 eV for Na 2 NiV 2 O 7 and 1.92 eV for Ag 2 NiV 2 O 7 , affirming their semiconductor properties. Further characterization was performed using density functional theory (DFT) and hybrid-DFT methods. These advanced techniques provide detailed understanding of the electronic structure and properties across different sodium–silver ratios. The computed electronic structures demonstrate the separation of the conduction band (CB) and valence band (VB) around the Fermi level, with bandgaps of 0.44 eV and 1.76 eV for Na 2 NiV 2 O 7 , and 0.56 eV and 1.60 eV for Ag 2 NiV 2 O 7 , as determined using the Perdew–Burke–Ernzerhof (PBE) and DFT+U methods, respectively. This comprehensive investigation offers valuable insights into the optical and electronic dynamics of nickel pyro-vanadate compounds, establishing a foundation for their potential applications in various fields, including optoelectronics, photocatalysis, and energy storage.

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Laboratory of Molecular Spectroscopy Modelling, Materials, Nanomaterials, Water and Environment, CERNE2D, Faculty of Science, Mohammed V University in Rabat, Rabat, Morocco

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Ayad, A., Benhsina, E., Guerraf, A.E. et al. Synthesis and Optical-Electronic Characterization of Nickel Pyro-Vanadate A 2 NiV 2 O 7 (A = Na, Ag) Semiconductors: Experimental, DFT, and Hybrid-DFT Approaches. J. Electron. Mater. (2024). https://doi.org/10.1007/s11664-024-11408-y

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Received : 30 April 2024

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Published : 12 September 2024

DOI : https://doi.org/10.1007/s11664-024-11408-y

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• Published: 06 January 2023

The first year of Nature Synthesis

Nature Synthesis volume  2 ,  page 1 ( 2023 ) Cite this article

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• Chemistry publishing
• Communicating chemistry
• Materials chemistry
• Chemical synthesis

As the journal celebrates its inaugural volume, we reflect on one year of content with highlights from 2022 and aspirations for the future.

At the outset, we envisaged that Nature Synthesis would publish articles on two main themes — target-oriented synthesis and method-oriented synthesis. The former, target-driven articles, report a final product of interest either for practical reasons, or to establish unknowns of the product’s chemical and physical properties to further our understanding. For method-oriented articles, the journey of making the molecule or material signifies the advance compared with the state-of-the-art. Now, looking back through Volume 1 , we recognize research articles on these themes, as well as an interweaving of both. Many examples spring to mind but here, we highlight a few.

Hu et al. reported the formation of γ-graphyne, which comprises an equal portion of sp - and sp 2 -hybridized carbon atoms 1 . A challenging allotrope of carbon to synthesize, γ-graphyne was made using reversible dynamic alkyne metathesis and by controlling the balance between kinetic and thermodynamic factors. Featured on the cover of this Issue, Wu et al. reported contra-helical iron( ii )-templated trefoil knots, which are synthesized by coaxially nesting a small multistranded helix within a larger reverse helix. These trefoil knots show topomechanically tuneable spin-crossover properties in the iron( ii ) centres. In both cases, the syntheses of these targets are impressive and, although these advances are at the forefront of the articles, the route to making them and the properties identified are also key.

On a method-oriented theme, Mateos et al. investigated the mechanism of light-driven [2 + 2] heterocycloadditions (Paternò–Büchi reactions) between indoles and ketones and used the knowledge gained about key intermediates to control the stereoselectivity of the reactions. As a result, diastereoisomers that were previously inaccessible could be prepared. In materials chemistry, Zhang et al. described a flux-assisted growth method for atomically thin materials (ATMs) including metal chalcogenides, oxides and oxyhalides 2 . Preparing high-quality ATMs can be difficult; however, using this route, a flux-crystallization mechanism enables precise control of their stoichiometry, and the confined reaction space guarantees the formation of ATMs. In the area of total synthesis, Ungarean et al. reported the development of a catalytic enantioselective hydroamination of benzene 3 . The chemical synthesis of aminoglycoside antibiotics is typically lengthy; however, this methodology enables the total synthesis of aminoglycoside (+)-ribostamycin in ten linear steps from benzene.

To celebrate our first anniversary, the editors of Nature Synthesis have curated a Collection of content published so far, in which we showcase the scientific areas and the variety of article types that typically feature in the journal.

We include in our Collection the Comment article by K. Barry Sharpless 4 , one of the laureates of the 2022 Nobel Prize in Chemistry. Entitled “Click chemistry connections for functional discovery” and co-authored by M. G. Finn and Hartmuth C. Kolb, the Comment explains how click chemistry involves the reaction of two molecules in a manner akin to “the satisfaction of easily connecting two objects with the snap of a push buckle”. A sketch from the lab notebook of Sharpless is featured — with molecules, drawn in ink, that have become emblematic of click chemistry over the past two decades. The simple and efficient nature of click reactions swiftly made them popular for the synthesis of small well-defined molecules, as well as extended materials, and it is not surprising that the Nobel committee recognized click chemistry this year. We congratulate all three laureates — Carolyn R. Bertozzi, Morten Meldal and K. Barry Sharpless — on their notable achievements.

The discovery of synthetic routes and the improvement of known methods are now benefiting from innovations in automation and machine learning. In several articles, these technology-enabled syntheses are described — including, but not limited to, a computer-driven strategy enabling the systematic discovery and evaluation of iterative sequences of organic reactions reported by Molga et al. 5 , and an automated carbohydrate synthesizer capable of preparing a library of bioactive oligosaccharides by Yao et al. 6 . This automated synthesizer rapidly assembles carbohydrates up to 1,080-mer in size, starting from monosaccharide building blocks.

In addition, the importance of sustainable methods — to synthesize molecules and materials, as well as degrade and recycle them — has featured in the articles published this year. Kim et al. reported a biocatalytic photoelectrochemical approach to use non-recyclable microplastics as electron feedstocks that are broken down to produce value-added oxidation products, while at the same time, accelerating redox biosynthetic reactions 7 . Thus, the approach combines environmental remediation and the sustainable synthesis of chemicals from solar energy.

A central aim of Nature Synthesis was to provide a venue for reporting the best synthetic papers in chemistry and materials science and, perusing Volume 1, these disciplines — that already come together in research laboratories — are brought together in the issues we have published. In achieving this, we thank our authors and referees for supporting Nature Synthesis by either choosing to publish with us or for peer-reviewing manuscripts with the rigour and constructive opinion that we require.

Looking forward to Volume 2, in addition to the breadth of topics seen in Volume 1, we are planning to highlight topics such as ammonia synthesis, automation in synthetic laboratories and hydrogen atom transfer for C( sp 3 )–H functionalization — watch this space!

Hu, Y. et al. Nat. Synth. 1 , 449–454 (2022).

Article   Google Scholar  

Zhang, P. et al. Nat. Synth. 1 , 864–872 (2022).

Ungarean, C. N. et al. Nat. Synth. 1 , 542–547 (2022).

Finn, M. G., Kolb, H. C. & Sharpless, K. B. Nat. Synth. 1 , 8–10 (2022).

Molga, K. et al. Nat. Synth. 1 , 49–58 (2022).

Yao, W. et al. Nat. Synth. 1 , 854–863 (2022).

Kim, J., Jang, J., Hilberath, T., Hollmann, F. & Park, C. B. Nat. Synth. 1 , 776–786 (2022).

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The first year of Nature Synthesis . Nat. Synth 2 , 1 (2023). https://doi.org/10.1038/s44160-022-00237-8

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Published : 06 January 2023

Issue Date : January 2023

DOI : https://doi.org/10.1038/s44160-022-00237-8

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