Science China Chemistry最新文献

{"title":"Upcycling of polyethylene terephthalate to 1,4-cyclohexanedimethanol in water","authors":"Shuhui Fang,&nbsp;Zhiwen Gao,&nbsp;Xinrui Shi,&nbsp;Min Zhang,&nbsp;Wei Zhang,&nbsp;Yue Liu","doi":"10.1007/s11426-024-2429-0","DOIUrl":"10.1007/s11426-024-2429-0","url":null,"abstract":"<div><p>The recycling of waste polyethylene terephthalate (PET), an extensively used polymer as plastic and fiber materials, has become an urgent topic due to the rapid generation and accumulation of plastic waste into the environment. Current chemical recycling approaches to depolymerize and convert PET into 1,4-cyclohexanedimethanol (CHDM), an important chemical in the production of advanced polyesters, predominantly use organic solvents, such as alcohols or dioxane. Herein, we developed an environmentally friendly and economically viable pathway for converting PET to CHDM using water as the solvent. In this process, PET is sequentially hydrolyzed in water, hydrogenated to 1,4-cyclohexane dicarboxylic acid (CHDA), and then reduced to CHDM. The PET conversion rate is self-enhanced in aqueous medium via acid-catalyzed hydrolysis by the generated CHDA intermediate. A Pd-based catalyst (e.g., Pd/C) selectively hydrogenates the arene ring of the PET monomer, terephthalic acid intermediate, and a Ru-Sn/C bimetallic catalyst reduces its COOH to CH₂OH group. At optimized reaction conditions, a complete conversion of PET and 80.1% yield of CHDM are obtained. Alternatively, this approach can also efficiently produce CHDA from PET, with a yield up to 86.4%.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 5","pages":"2101 - 2109"},"PeriodicalIF":10.4,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143919023","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}

{"title":"Multicomponent polymerization of elemental sulfur, difluoromethylene phosphobetaine and aryl silyl ethers toward aromatic poly(O,O′-monothiocarbonate)s","authors":"Yongjiang Yu,&nbsp;Rongrong Hu,&nbsp;Ben Zhong Tang","doi":"10.1007/s11426-024-2421-3","DOIUrl":"10.1007/s11426-024-2421-3","url":null,"abstract":"<div><p>Polythiocarbonates with similar structures to polycarbonates, have emerged as a group of promising sulfur-containing polymers with a range of practical applications, taking advantages of their excellent optical properties, good thermal stability and film-forming ability, and so on. However, the synthesis of polythiocarbonates generally suffered from mixed isomeric structures of repeating units, and hazardous sulfur-containing reagents. In this work, an efficient multicomponent reaction of elemental sulfur, difluoromethylene phosphobetaine (PDFA), and aryl silyl ethers was designed with the assistance of organic base 7-methyl-1,5,7-triazabicyclo[4.4.0]dec-5-ene (MTBD) to produce 12 kinds of <i>O</i>,<i>O</i>′-monothiocarbonate compounds in up to 93% yields, taking advantages of the unique chemical property of difluorocarbene, and the deprotection of silyl group by F⁻ generated from PDFA. Most importantly, the MTBD-assisted multicomponent polymerization of bis(aryl silyl ether)s, elemental sulfur, and PDFA was developed, affording 12 kinds of poly(<i>O</i>,<i>O</i>′-monothiocarbonate)s with well-defined structures, high <i>M</i>_ws of up to 16900 g/mol and high yields (up to 99%). These poly(<i>O</i>,<i>O</i>′-monothiocarbonate)s possessed good film-forming properties and thermal stability, high light refractive indices and transmittance. The facile synthesis of these polymonothiocarbonates might pave the way for the development of promising sulfur-containing polymer materials.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 5","pages":"1970 - 1979"},"PeriodicalIF":10.4,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143919019","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}

{"title":"Smart windows with high optical transparency and structural color","authors":"Youtong Wu,&nbsp;Xueting Li,&nbsp;Yiwen Li,&nbsp;Hao Wang,&nbsp;Yuqi Zhang,&nbsp;Xihua Lu","doi":"10.1007/s11426-024-2423-0","DOIUrl":"10.1007/s11426-024-2423-0","url":null,"abstract":"<div><p>In recent years, thermochromic smart windows have played an important role in enhancing energy efficiency and contributing to carbon neutrality in building energy consumption. However, thermal-shielding smart windows with high visible light modulation and structural colors are rarely reported. This study focuses on the development of thermochromic smart windows utilizing poly (<i>N</i>-isopropylacrylamide) (PNIPAm)-based nanogels, which exhibit dynamic solar modulation and high visible light transmission without additional energy input. Unlike traditional electrochromic materials such as tungsten trioxide, these smart windows achieve structural color states through the self-assembly of nanogels, eliminating the need for inorganic materials. The fabricated hydrogel contains thermo-responsive poly(<i>N</i>-isopropylacrylamide-random-acrylic acid-random-<i>N-tert</i>-butyl acrylamide) P(NIPAm-r-AA-r-TBA) (PNTA) nanogels with tunable phase transition temperatures (<i>T</i>_p) that align with ambient conditions. These smart windows demonstrate excellent stability over 100 heating-cooling cycles and significant temperature regulation, achieving an indoor temperature modulation of 10 °C and energy savings of 14.24 KJ m⁻³ compared with normal windows. The production process is simple and scalable, making it feasible for industrial applications. Furthermore, these smart windows offer additional functionalities such as information encryption, adding value to their practical application.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 5","pages":"2017 - 2026"},"PeriodicalIF":10.4,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143919022","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}

{"title":"Adding new dimension to non-directed C(sp3)–H functionalizations","authors":"Konstantin P. Bryliakov","doi":"10.1007/s11426-024-2431-3","DOIUrl":"10.1007/s11426-024-2431-3","url":null,"abstract":"","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 4","pages":"1215 - 1217"},"PeriodicalIF":10.4,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716830","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}

{"title":"Three-dimensional covalent organic frameworks with self-catenated topology for methane storage","authors":"Jiandong Pang,&nbsp;Xian-He Bu","doi":"10.1007/s11426-024-2476-x","DOIUrl":"10.1007/s11426-024-2476-x","url":null,"abstract":"","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 3","pages":"808 - 809"},"PeriodicalIF":10.4,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s11426-024-2476-x.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475124","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}

{"title":"Recent progress in metal-organic frameworks (Part II—material application)","authors":"Jiandong Pang,&nbsp;Wentao Jiang,&nbsp;Xue-Wen Zhang,&nbsp;Hao-Long Zhou,&nbsp;Yuxiu Sun,&nbsp;Wei Gong,&nbsp;Bin Wang,&nbsp;Fuyin Ma,&nbsp;Linwei He,&nbsp;Long Chen,&nbsp;Qiang Chen,&nbsp;He-Qi Zheng,&nbsp;Yuanjing Cui,&nbsp;Wen-Jie Shi,&nbsp;Chao Zhang,&nbsp;Mei Wang,&nbsp;Yue-Biao Zhang,&nbsp;Jie-Peng Zhang,&nbsp;Chongli Zhong,&nbsp;Yong Cui,&nbsp;Shuao Wang,&nbsp;Jian-Rong Li,&nbsp;Guodong Qian,&nbsp;Tong-Bu Lu,&nbsp;Huan Pang,&nbsp;Xian-He Bu","doi":"10.1007/s11426-024-2458-3","DOIUrl":"10.1007/s11426-024-2458-3","url":null,"abstract":"<div><p>As a class of functional crystalline porous materials, metal-organic frameworks (MOFs) gained rapid development in the past three decades and a large number of MOFs with ordered structures, high surface areas, and functionalized channels have been investigated. MOFs and MOF-derived/composite materials show great potential in many application fields. In this review, we discussed the main applications of MOFs and MOF-derived/composite materials in small molecule storage, separation, luminescence, sensing, multitype catalysis, and energy storage. In addition, challenges and problems in the future research of MOFs-related fields are also discussed.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 5","pages":"1642 - 1702"},"PeriodicalIF":10.4,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143919021","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}

{"title":"Engineering high-performance chemiluminescent probes via enzymatic pocket targeting: high-throughput screening for ultralong afterglow imaging of orthotopic hepatocellular carcinoma","authors":"Shuai Huang,&nbsp;Shuaige Bai,&nbsp;Ting Luo,&nbsp;Bin Feng,&nbsp;Min Liu,&nbsp;Fan Zheng,&nbsp;Shuang Huang,&nbsp;Yanpeng Fang,&nbsp;Dan Ding,&nbsp;Wenbin Zeng","doi":"10.1007/s11426-024-2296-6","DOIUrl":"10.1007/s11426-024-2296-6","url":null,"abstract":"<div><p>Hepatocellular carcinoma (HCC) is a highly aggressive liver malignancy and the main form of liver cancer. Early diagnosis and treatment of HCC can effectively reduce mortality. Carboxylesterase (CE)-specific detection and imaging can be used for early diagnosis and image-guided surgical of HCC. However, traditional optical probes suffer from poor selectivity and low imaging signal-to-noise ratio. Here, we have constructed a series of chemiluminescent probes for carboxylesterase detection based on the strategy of enzymatic pocket-oriented steric tailoring techniques. The probes with different unique and excellent properties have been obtained through the structure-based steric hindrance adjustment on the recognition site. Here, <b>CE-2</b> has been successfully used for high-throughput screening of rapid carboxylesterase inhibitors due to its extremely low detection limit (2.5 × 10⁻⁴ U mL⁻¹) and fast recognition ability. <b>CE-3</b> has been successfully used for image-guided surgery of orthotopic hepatocellular carcinoma due to its ultra-long chemiluminescence imaging (over 12 h) of hepatocellular carcinoma. This study may promote advances in the rapid detection and screening of inhibitory drugs for CE and the field of surgical navigation in HCC.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 3","pages":"1175 - 1184"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475104","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}

{"title":"Thermoresponsive helical dendronized poly(arylacetylene)s: modulating the dynamic chirality","authors":"Xueting Lu,&nbsp;Lei Wang,&nbsp;Liangxuan Ren,&nbsp;Wen Li,&nbsp;Afang Zhang","doi":"10.1007/s11426-024-2302-8","DOIUrl":"10.1007/s11426-024-2302-8","url":null,"abstract":"<div><p>Helical poly(arylacetylene)s have formed an intriguing class of polymers, whose chiralities are dynamic and liable to external stimuli. By combining dendronized polymer topology with dendritic oligoethylene glycols (OEGs), we here report on synthesis of a homologous series of thermoresponsive dendronized poly(arylacetylene)s with either poly(phenyl acetylene) or poly (naphthalene acetylene) as the backbones, and investigate tunability of their helical conformations. These polymers carry dendritic OEG pendants with either methoxyl- or ethoxyl-terminals to tune their unprecedent thermoresponsive behaviors, and at the same time, dendritic shielding plays an important role in mediating their thermal phase transition temperatures. Helicity of these polymers is originated from the chiral alanine or phenylalanine moieties within the dendritic pendants, which can be tailored through manipulating solvation in different organic solvents or via thermal dehydration and collapse in water. Furthermore, achiral additives such as linear or dendritic OEGs and benzene derivatives can act similarly as thermal dehydration to induce chirality transitions of these polymers in aqueous phase through interplay competitions between the additives and the polymers against their hydration.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 4","pages":"1486 - 1496"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716761","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}

{"title":"Sulfhydryl-modified zeolite A with exceptional strontium adsorption selectivity","authors":"Lingyi Li,&nbsp;Lanxing Ren,&nbsp;Dong Wang,&nbsp;Junchang Chen,&nbsp;Qi Guo,&nbsp;Yuting Zhao,&nbsp;Fuqiang Zhao,&nbsp;Linwei He,&nbsp;Jie Li,&nbsp;Wenqi Zhang,&nbsp;Lijuan Song,&nbsp;Long Chen,&nbsp;Lixi Chen,&nbsp;Bin Wang,&nbsp;Lin Zhu,&nbsp;Tao Duan,&nbsp;Zhifang Chai,&nbsp;Shuao Wang","doi":"10.1007/s11426-024-2267-2","DOIUrl":"10.1007/s11426-024-2267-2","url":null,"abstract":"<div><p>Efficient removal of trace radiostrontium from contaminated highly saline wastewater, such as seawater, remains a critical but challenging task due to the coexistence of large excess of hard cations like Na⁺, K⁺, Mg²⁺ and particularly Ca²⁺, which shares similar physicochemical properties with Sr²⁺. Herein, we successfully boosted the selectivity by a sulfhydryl-functionalized NaA zeolite (SH-NaA) <i>via</i> ion exchange coupled with reinforced soft-soft interactions between sulfhydryl groups and Sr²⁺. Remarkably, SH-NaA achieved a 99.8% removal efficiency of Sr²⁺ in the presence of a tenfold excess of Ca²⁺, with a distribution coefficient (<i>K</i>_<i>d</i>) of 4.98×10⁵ mL/g. The effectiveness of SH-NaA in accurately capturing Sr²⁺ was further validated by its superior dynamic adsorption performance in natural seawater compared to pristine NaA zeolite. Batch experiments highlighted SH-NaA’s exceptional Sr²⁺ removal efficiency (<i>q</i>_<i>m</i> = 233.36 mg/g), rapid adsorption kinetics (1 min), superior decontamination depth (<i>K</i>_<i>d</i> = 6.71×10⁵ mL/g), and robust irradiation stability (400 kGy γ-ray). X-ray photoelectron spectroscopy (XPS) and <i>in situ</i> Fourier-transform infrared (FTIR) analyses underscored the pivotal role of sulfhydryl groups in Sr²⁺ capture. Density functional theory (DFT) calculations revealed that the sulfhydryl-functionalized NaA zeolite exhibits the best selectivity toward Sr²⁺, with an interaction energy of −2.55 eV. These findings demonstrate that organic group functionalized zeolites hold significant promise for environmental remediation applications.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 5","pages":"1847 - 1858"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143918978","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}

{"title":"Growth behavior and electronic regulation of Pt on various Mo-based supports for hydrogen evolution electrocatalysis","authors":"Lulu Chen,&nbsp;Yichao Huang,&nbsp;Jiajun Wang,&nbsp;Meihong Liao,&nbsp;Zhiyuan Liu,&nbsp;Meiqi Liu,&nbsp;Hanqing Cai,&nbsp;Lin Wang,&nbsp;Lidong Gao,&nbsp;Dawei Hu,&nbsp;Lianming Zhao,&nbsp;Ning Pu,&nbsp;Zhuangjun Fan","doi":"10.1007/s11426-024-2324-8","DOIUrl":"10.1007/s11426-024-2324-8","url":null,"abstract":"<div><p>Insight into the growth behavior and electronic regulation of platinum (Pt) on various transition metal supports is paramount in developing high-performing electrocatalysts for hydrogen evolution reactions (HER). Herein, we studied the influence of molybdenum-based supports (MoX, X = C, N, P, and S) on the growth behavior and electronic regulation of Pt. We found that the formation energy variations between Pt single atom and clusters on MoX supports play a pivotal role in the growth behavior of Pt. Moreover, the electronic regulation of Pt induced by metal-support interaction may reflect the valence changes of Pt in Pt-MoX/C. The Pt-MoC/C catalyst with a moderate valence state of Pt exhibits the best HER activity with an overpotential of 12.0 mV at 10 mA cm⁻² and a mass activity of 27.1 A mg_Pt⁻¹, 12.3 times as high as that of commercial 20 wt% Pt/C. This work provides constructive guidance for the design of high-performance HER catalysts.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 5","pages":"1837 - 1846"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143918979","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}