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Chemical and engineering bases for green H2O2 production and related oxidation and ammoximation of olefins and analogues 绿色 H2O2 生产以及烯烃和类似物的相关氧化和胺氧化的化学和工程基础
IF 20.6 1区 综合性期刊
National Science Review Pub Date : 2024-07-17 DOI: 10.1093/nsr/nwae243
Minghua Qiao, Xinggui Zhou, Zexue Du, Peng Wu, Baoning Zong
{"title":"Chemical and engineering bases for green H2O2 production and related oxidation and ammoximation of olefins and analogues","authors":"Minghua Qiao, Xinggui Zhou, Zexue Du, Peng Wu, Baoning Zong","doi":"10.1093/nsr/nwae243","DOIUrl":"https://doi.org/10.1093/nsr/nwae243","url":null,"abstract":"Plastics, fibers, and rubber are three mainstream synthetic materials that are essential to our daily life and contribute significantly to the quality of our life. The production of the monomers of these synthetic polymers usually involves oxidation or ammoximation reactions of olefins and analogues. However, the utilization of the C, O, and N atoms in current industrial processes is less than 80%, which represents the most environmentally polluting processes for the production of basic chemicals. Through innovation and integration of catalytic materials, new reaction pathways, and reaction engineering, Research Institute of Petroleum Processing, Sinopec Co., Ltd. (RIPP) and its collaborators have developed unique H2O2-centered oxidation/ammoximation technologies of olefins and analogues, which has formed a ¥500 billion emerging industry and driven trillions of downstream industries. The chemical and engineering bases of the production technologies mainly involve the integration of slurry-bed reactors and microsphere catalysts to enhance H2O2 production, H2O2 propylene/chloropropylene epoxidation for the production of propylene oxide (PO)/epichlorohydrin (ECH), and integration of H2O2 cyclohexanone ammoximation and membrane separation to innovate the caprolactam production process. This review briefly summarizes the whole process from the acquisition of scientific knowledge to the formation of an industrial production technology by RIPP. Moreover, the scientific frontiers of H2O2 production and related oxidation/ammoximation processes of olefins and analogues are reviewed, and new technological growth points are envisaged, aiming at keeping China as one of the leaders in the development of the science and technologies in H2O2 production and utilization.","PeriodicalId":18842,"journal":{"name":"National Science Review","volume":"24 1","pages":""},"PeriodicalIF":20.6,"publicationDate":"2024-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141737139","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Fast selective edge-enhanced imaging with topological chiral lamellar superstructures 利用拓扑手性层状超结构实现快速选择性边缘增强成像
IF 20.6 1区 综合性期刊
National Science Review Pub Date : 2024-07-15 DOI: 10.1093/nsr/nwae247
Wen Chen, Dong Zhu, Si-Jia Liu, Yi-Heng Zhang, Lin Zhu, Chao-Yi Li, Shi-Jun Ge, Peng Chen, Wan-Long Zhang, Xiao-Cong Yuan, Yan-Qing Lu
{"title":"Fast selective edge-enhanced imaging with topological chiral lamellar superstructures","authors":"Wen Chen, Dong Zhu, Si-Jia Liu, Yi-Heng Zhang, Lin Zhu, Chao-Yi Li, Shi-Jun Ge, Peng Chen, Wan-Long Zhang, Xiao-Cong Yuan, Yan-Qing Lu","doi":"10.1093/nsr/nwae247","DOIUrl":"https://doi.org/10.1093/nsr/nwae247","url":null,"abstract":"Edge detection is a fundamental operation for feature extraction in the image processing. All-optical method arouses growing interest owing to its ultra-fast speed, low energy consumption and parallel computation. However, current optical edge detection is generally limited to static devices and fixed functionality. Herein, we propose a fast-switchable scheme based on a ferroelectric liquid crystal topological structure. The self-assembled chiral lamellar superstructure, directed by the azimuthally-variant photo-alignment agent, can be dynamically controlled by the polarity of external electric field, and respectively generates the vector beams with nearly orthogonal polarization distribution. Even after thousands of cycles, horizontal and vertical edges of the object are selectively enhanced with an ultra-fast switching time of about 57 μs. Broadband edge-enhanced imaging is efficiently demonstrated. This work extends the ingenious building of topological heliconical superstructures, and offers an important glimpse into their potentials in the emerging frontiers of optical computing for artificial intelligence.","PeriodicalId":18842,"journal":{"name":"National Science Review","volume":"16 1","pages":""},"PeriodicalIF":20.6,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141737141","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A highly-selective biomimetic potassium channel 高选择性生物仿生钾通道
IF 20.6 1区 综合性期刊
National Science Review Pub Date : 2024-07-14 DOI: 10.1093/nsr/nwae242
Junliang Zhu, Hu Qiu, Wanlin Guo
{"title":"A highly-selective biomimetic potassium channel","authors":"Junliang Zhu, Hu Qiu, Wanlin Guo","doi":"10.1093/nsr/nwae242","DOIUrl":"https://doi.org/10.1093/nsr/nwae242","url":null,"abstract":"Reproducing the outstanding selectivity achieved by biological ion channels in artificial channel systems can revolutionize applications ranging from membrane filtration to single-molecule sensing technologies, but achieving this goal remains a challenge. Herein, inspired by the selectivity filter structure of the KcsA potassium channel, we propose a design of biomimetic potassium nanochannels by functionalizing the wall of carbon nanotubes with an array of arranged carbonyl oxygen atoms. Our extensive molecular dynamics simulations show that the biomimetic nanochannel exhibits a high K+ permeation rate and meanwhile a high K+/Na+ selectivity ratio. The free energy calculations suggest that the low Na+ permeability is the result of the higher energy barrier for Na+ than K+ at the channel entrance and ion binding sites. In addition, reducing the number of ion binding sites leads to an increase in the permeation rate but a decrease in the selectivity. These findings not only hold promise for the design of high-performance membranes but also help understand the mechanism of selective ion transport in biological ion channels.","PeriodicalId":18842,"journal":{"name":"National Science Review","volume":"32 1","pages":""},"PeriodicalIF":20.6,"publicationDate":"2024-07-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141610742","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mantle plume trail beneath the ca. 1.1 Ga North American Midcontinent rift revealed by magnetotelluric data 由磁力线数据揭示的约 1.1 Ga 北美洲中大陆裂谷下的地幔羽流轨迹磁辐射数据揭示的 1.1 Ga 北美大陆中部裂谷
IF 20.6 1区 综合性期刊
National Science Review Pub Date : 2024-07-12 DOI: 10.1093/nsr/nwae239
Wule Lin, Adam Schultz, Bo Yang, Lyal B Harris, Xiangyun Hu
{"title":"Mantle plume trail beneath the ca. 1.1 Ga North American Midcontinent rift revealed by magnetotelluric data","authors":"Wule Lin, Adam Schultz, Bo Yang, Lyal B Harris, Xiangyun Hu","doi":"10.1093/nsr/nwae239","DOIUrl":"https://doi.org/10.1093/nsr/nwae239","url":null,"abstract":"Whilst the 1.1 Ga North American Midcontinent Rift system (MCR) is formed in association with the Keweenaw mantle plume, the absence of a northern third rift arm or aulacogen (a general characteristic of mantle plumes) has previously not been well understood. To help clarify this unusual plume-rift relationship and to better establish the region affected by the Keweenaw mantle plume, we present the first electrical resistivity model of the MCR derived from three-dimensional inversion of EarthScope USArray and Lithoprobe magnetotelluric (MT) data, extending northwards into the Archean Superior Province. Our model shows a prominent highly conductive anomaly trending NW-SE at the base of Western Superior's cratonic lithospheric mantle, cross-cutting and extending for over 300 km on both sides of the western rift branch. We propose that this anomaly reflects the ancient signature of a plume trail, resulting from metasomatism and/or partial melting of the sulfide-rich basal lithospheric mantle during impingement of the Keweenaw mantle plume.","PeriodicalId":18842,"journal":{"name":"National Science Review","volume":"49 1","pages":""},"PeriodicalIF":20.6,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141610740","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Electron-injection-engineering induced dual-phase MoO2.8F0.2/MoO2.4F0.6 heterostructure for magnesium storage 用于镁储存的电子注入工程诱导双相 MoO2.8F0.2/MoO2.4F0.6 异质结构
IF 20.6 1区 综合性期刊
National Science Review Pub Date : 2024-07-12 DOI: 10.1093/nsr/nwae238
Weixiao Wang, Fangyu Xiong, Shaohua Zhu, Mengyu Yan, Xiaobin Liao, Kesong Yu, Lianmeng Cui, Jinghui Chen, Junjun Wang, Ruoqi Lan, Jun Xie, Qinyou An, Liqiang Mai
{"title":"Electron-injection-engineering induced dual-phase MoO2.8F0.2/MoO2.4F0.6 heterostructure for magnesium storage","authors":"Weixiao Wang, Fangyu Xiong, Shaohua Zhu, Mengyu Yan, Xiaobin Liao, Kesong Yu, Lianmeng Cui, Jinghui Chen, Junjun Wang, Ruoqi Lan, Jun Xie, Qinyou An, Liqiang Mai","doi":"10.1093/nsr/nwae238","DOIUrl":"https://doi.org/10.1093/nsr/nwae238","url":null,"abstract":"Rechargeable magnesium batteries (RMBs) have received incremental attention due to their high volumetric capacity and safety. Nevertheless, the sluggish diffusion kinetics of highly polarized Mg2+ in host lattices severely hinders the development of RMBs. Herein, we report an electron injection strategy for modulating Mo 4d-orbital splitting manner and firstly fabricate a dual-phase MoO2.8F0.2/MoO2.4F0.6 heterostructure to accelerate Mg2+ diffusion. The electron injection strategy triggers weak Jahn-Teller distortion in MoO6 octahedra and reorganization of the Mo 4d-orbital, leading to a partial phase transition from orthorhombic phase MoO2.8F0.2 to cubic phase MoO2.4F0.6. As a result, the designed heterostructure generates a built-in electric field, simultaneously improves its electronic conductivity and ionic diffusivity by at least one order of magnitude compared to MoO2.8F0.2 and MoO2.4F0.6. Importantly, the assembled MoO2.8F0.2/MoO2.4F0.6//Mg full cell exhibits a remarkable reversible capacity of 172.5 mA h g−1 at 0.1 A g−1, pushing forward the orbital-scale manipulation for high-performance RMBs.","PeriodicalId":18842,"journal":{"name":"National Science Review","volume":"41 1","pages":""},"PeriodicalIF":20.6,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141610743","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Understanding the interfacial water structure in electrocatalysis 了解电催化过程中的界面水结构
IF 20.6 1区 综合性期刊
National Science Review Pub Date : 2024-07-12 DOI: 10.1093/nsr/nwae241
Guoshuai Shi, Tingyu Lu, Liming Zhang
{"title":"Understanding the interfacial water structure in electrocatalysis","authors":"Guoshuai Shi, Tingyu Lu, Liming Zhang","doi":"10.1093/nsr/nwae241","DOIUrl":"https://doi.org/10.1093/nsr/nwae241","url":null,"abstract":"The structure of interfacial water molecules plays a crucial role in modulating the electrochemical surface kinetics. This article provides an in-depth understanding of the water molecule structure inside the double layer and its main influencing factors at the molecular scale.","PeriodicalId":18842,"journal":{"name":"National Science Review","volume":"36 1","pages":""},"PeriodicalIF":20.6,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141614684","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Pan-cancer integrative analyses dissect the remodeling of endothelial cells in human cancers 泛癌症综合分析剖析人类癌症中内皮细胞的重塑
IF 20.6 1区 综合性期刊
National Science Review Pub Date : 2024-07-10 DOI: 10.1093/nsr/nwae231
Jinhu Li, Dongfang Wang, Fei Tang, Xinnan Ling, Wenjie Zhang, Zemin Zhang
{"title":"Pan-cancer integrative analyses dissect the remodeling of endothelial cells in human cancers","authors":"Jinhu Li, Dongfang Wang, Fei Tang, Xinnan Ling, Wenjie Zhang, Zemin Zhang","doi":"10.1093/nsr/nwae231","DOIUrl":"https://doi.org/10.1093/nsr/nwae231","url":null,"abstract":"Therapeutics targeting tumor endothelial cells (TECs) have been explored for decades, with only suboptimal efficacy achieved, partly due to an insufficient understanding of the TEC heterogeneity across cancer patients. We integrated single-cell RNA-seq data of 575 cancer patients from 19 solid tumor types, comprehensively charting the TEC phenotypic diversities. Our analyses uncovered underappreciated compositional and functional heterogeneity in TECs from a pan-cancer perspective. Two subsets, CXCR4+ tip cells and SELE+ veins, represented the prominent angiogenic and proinflammatory phenotypes of TECs, respectively. They exhibited distinct spatial organization patterns, and compared to adjacent non-tumor tissues, tumor tissue showed an increased prevalence of CXCR4+ tip cells, yet with SELE+ veins depleted. Such functional and spatial characteristics underlie their differential associations with the response of anti-angiogenic therapies and immunotherapies. Our integrative resources and findings open new avenues to understand and clinically intervene in the tumor vasculature.","PeriodicalId":18842,"journal":{"name":"National Science Review","volume":"9 1","pages":""},"PeriodicalIF":20.6,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141610744","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Technologies for investigating single-molecule chemical reactions 研究单分子化学反应的技术
IF 20.6 1区 综合性期刊
National Science Review Pub Date : 2024-07-10 DOI: 10.1093/nsr/nwae236
Chunyan Gao, Qinghua Gao, Cong Zhao, Yani Huo, Zhizhuo Zhang, Jinlong Yang, Chuancheng Jia, Xuefeng Guo
{"title":"Technologies for investigating single-molecule chemical reactions","authors":"Chunyan Gao, Qinghua Gao, Cong Zhao, Yani Huo, Zhizhuo Zhang, Jinlong Yang, Chuancheng Jia, Xuefeng Guo","doi":"10.1093/nsr/nwae236","DOIUrl":"https://doi.org/10.1093/nsr/nwae236","url":null,"abstract":"Single molecules, the smallest independently stable units in the material world, serve as the fundamental building blocks of matters. Among different branches of single-molecule sciences, single-molecule chemical reactions, by revealing the behavior and properties of individual molecules at the molecular scale, are particularly attractive because they can advance the understanding of chemical reaction mechanisms and help to address key scientific problems in broad fields such as physics, chemistry, biology, and materials science. This review provides a timely, comprehensive overview of single-molecule chemical reactions based on various technical platforms such as scanning probe microscopy, single-molecule junction, single nanostructure, single-molecule fluorescence detection, and crossed molecular beam. We present multidimensional analyses of single-molecule chemical reactions, offering new perspectives for research in different areas like photocatalysis/electrocatalysis, organic reactions, surface reactions, and biological reactions. Finally, we discuss the opportunities and challenges in this thriving field of single-molecule chemical reaction.","PeriodicalId":18842,"journal":{"name":"National Science Review","volume":"26 1","pages":""},"PeriodicalIF":20.6,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141588428","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
New ionizable lipids reduce the lipid-to-mRNA ratio for base editing. 新的可离子化脂质降低了碱基编辑中脂质与核糖核酸的比例。
IF 16.3 1区 综合性期刊
National Science Review Pub Date : 2024-07-09 eCollection Date: 2024-08-01 DOI: 10.1093/nsr/nwae224
Shuliang Gao, Qiaobing Xu
{"title":"New ionizable lipids reduce the lipid-to-mRNA ratio for base editing.","authors":"Shuliang Gao, Qiaobing Xu","doi":"10.1093/nsr/nwae224","DOIUrl":"10.1093/nsr/nwae224","url":null,"abstract":"","PeriodicalId":18842,"journal":{"name":"National Science Review","volume":"11 8","pages":"nwae224"},"PeriodicalIF":16.3,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11310581/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141917169","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Seawater barium and sulfide removal improved marine habitability for the Cambrian Explosion of early animals 海水钡和硫化物的去除改善了寒武纪早期动物大爆发的海洋适居性
IF 20.6 1区 综合性期刊
National Science Review Pub Date : 2024-07-08 DOI: 10.1093/nsr/nwae237
Wei Wei, Lin-Hui Dong, Shuhai Xiao, Yi- Bo Lin, Lingang Xu, Guang-Yi Wei, Wenzhong Wang, Lan-Lan Tian, Hai-Zhen Wei, Fang Huang
{"title":"Seawater barium and sulfide removal improved marine habitability for the Cambrian Explosion of early animals","authors":"Wei Wei, Lin-Hui Dong, Shuhai Xiao, Yi- Bo Lin, Lingang Xu, Guang-Yi Wei, Wenzhong Wang, Lan-Lan Tian, Hai-Zhen Wei, Fang Huang","doi":"10.1093/nsr/nwae237","DOIUrl":"https://doi.org/10.1093/nsr/nwae237","url":null,"abstract":"An increase in atmospheric pO2 has been proposed as a trigger of the Cambrian Explosion at ∼539–514 Ma, but the mechanistic linkage remains unclear. To gain insights into marine habitability for the Cambrian Explosion, we analyzed excess Ba contents (Baexcess) and isotope compositions (δ138Baexcess) of ∼521-Myr-old metalliferous black shales in South China. The δ138Baexcess values vary within a large range, and show a negative logarithmic correlation with Baexcess, suggesting a major (>99%) drawdown of oceanic Ba inventory via barite precipitation. Spatial variations in Baexcess and δ138Baexcess indicate Ba removal was driven by sulfate availability ultimately derived from the upwelling of deep seawaters. Global oceanic oxygenation across the Ediacaran-Cambrian transition may have increased the sulfate reservoir via oxidation of sulfide and concurrently decreased the Ba reservoir by barite precipitation. The removal of both H2S and Ba that are deleterious to animals could have improved marine habitability for early animals.","PeriodicalId":18842,"journal":{"name":"National Science Review","volume":"30 1","pages":""},"PeriodicalIF":20.6,"publicationDate":"2024-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141586107","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","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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