Science China Chemistry最新文献_第3页

Guest-induced topological transformation and near-infrared photothermal conversion featuring the Cp*Rh unit via coordination-driven self-assembly

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2304-9

Xin-Yu Wang, Qiu-Shui Mu, Xiang Gao, Guo-Xin Jin

{"title":"Guest-induced topological transformation and near-infrared photothermal conversion featuring the Cp*Rh unit via coordination-driven self-assembly","authors":"Xin-Yu Wang, Qiu-Shui Mu, Xiang Gao, Guo-Xin Jin","doi":"10.1007/s11426-024-2304-9","DOIUrl":"10.1007/s11426-024-2304-9","url":null,"abstract":"<div><p>Herein, we perform a topological transformation by guest induction, converting [2]catenane <b>Rh-1</b> into the <b>Rh-3</b> molecular figure-of-eight. The transformation involves the interaction of longer <i>π</i>-acceptor half-sandwich Rh<sup>III</sup> bimetallic building block <b>B1</b> [(Cp*Rh)<sub>2</sub>(TPPHZ)](OTf)<sub>4</sub> and <i>π</i>-donor bipyridyl ligands 4,4′-bis((pyridin-4-ylthio)methyl)-1,1′-biphenyl with four molecules of pyrene under ambient temperature in high yields. Intriguingly, despite the involvement of a single pyrene molecule in modifying [2]catenane <b>Rh-2</b> by transitioning <b>B1</b> to <b>B2</b>, the underlying skeleton of <b>Rh-2</b> remains unaltered. Furthermore, we explored the application of these substances before and after the reaction for near-infrared (NIR) photothermal conversion. Through meticulous structural analysis, the <i>π</i>–<i>π</i> stacking interactions play a pivotal role in stabilizing the abovementioned structures, enhancing the nonradiative transitions and initiating photothermal conversion in solution. Based on the results, the introduction of pyrene significantly intensified the <i>π</i>–<i>π</i> stacking interactions but diminished the electron density between the adjacent NDI units, leading to a decrease in the NIR photothermal conversion efficiency (from 58.29% to 51.60%). In this study, an innovative approach is introduced for fabricating valuable half-sandwich-structured NIR photothermal conversion materials, and this research has promising prospects for enhancing the field of materials science with potential candidates for future development.</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":"1345 - 1354"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716752","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

A versatile synthetic strategy towards rare earth based metal-organic frameworks

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2322-9

Quan Shi, Yun-Hao Xu, Ming-Hui Chen, Peng Zhao, Wen-Bo Deng, Ji Xiong, Kai Guo, Ya-Qing Feng, Bao Zhang

{"title":"A versatile synthetic strategy towards rare earth based metal-organic frameworks","authors":"Quan Shi, Yun-Hao Xu, Ming-Hui Chen, Peng Zhao, Wen-Bo Deng, Ji Xiong, Kai Guo, Ya-Qing Feng, Bao Zhang","doi":"10.1007/s11426-024-2322-9","DOIUrl":"10.1007/s11426-024-2322-9","url":null,"abstract":"<div><p>Rare earth metal-organic frameworks (RE-MOFs) have drawn wide attention owing to diverse network structures and various application prospects. However, due to the unpredictable formation of the nodes, it is still challenging to design novel RE-MOFs. A novel versatile strategy was developed employing a RE-acetate complex (RE<sub>2</sub>(CH<sub>3</sub>COO)<sub>6</sub>·4H<sub>2</sub>O) as a precursor to construct RE-MOFs. 2D RE-MOFs (RE-DBP) and 3D RE-MOFs (RE-TCPP) could be obtained by using dicarboxylic porphyrin ligands H<sub>2</sub>DBP and tetracarboxylic porphyrin ligands H<sub>2</sub>TCPP, respectively. Ten RE-MOFs were further synthesized to verify the universality of the methodology. Highly crystalline RE-MOFs could also be prepared at room temperature via the developed strategy, which could significantly promote large-scale preparation and practical application of RE-MOFs. As proof of the concept, the performance of porphyrin-based RE-MOFs was investigated in the photocatalytic cycloaddition of CO<sub>2</sub> with epoxides. Among the RE-DBP(Co) MOFs, Tb-DBP(Co) exhibited the best photocatalytic performance, which was also greater than that of the corresponding 3D MOF Tb-TCPP(Co) due to the optimal 2D structure and thus the accelerated photogenerated charge separation and transfer process. This work not only provides a novel versatile strategy to design and develop RE-MOFs, but also proposes a promising approach for the potential bulk production of RE-MOFs at room temperature.</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":"1362 - 1371"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716765","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-selectivity electroreduction of low-concentration CO2 with large concentration fluctuation

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2307-y

Mengyu Qi, Yanbin Ma, Chao Zhang, Bingwei Li, Xueqing Yang, Zhaolin Shi, Simeng Liu, Changhua An, Jiqing Jiao, Tongbu Lu

{"title":"High-selectivity electroreduction of low-concentration CO2 with large concentration fluctuation","authors":"Mengyu Qi, Yanbin Ma, Chao Zhang, Bingwei Li, Xueqing Yang, Zhaolin Shi, Simeng Liu, Changhua An, Jiqing Jiao, Tongbu Lu","doi":"10.1007/s11426-024-2307-y","DOIUrl":"10.1007/s11426-024-2307-y","url":null,"abstract":"<div><p>Electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) has been regarded as one of the most promising solutions to achieving “zero carbon emission”. In most of the CO<sub>2</sub>RR-related studies, high-purity CO<sub>2</sub> has been employed as the feed gas; however, in practice, CO<sub>2</sub> is generally emitted in low concentrations, so it is of great significance to realize high-selectivity electroreduction of low-concentration CO<sub>2</sub> with large concentration fluctuation. In this work, we constructed a dual-active-site catalyst and successfully achieved CO<sub>2</sub> local enrichment and conversion for low-concentration CO<sub>2</sub>. <i>Operando</i> experiments reveal that the catalyst has one type of site for activating CO<sub>2</sub> and one type of site for binding the reaction intermediates. The dual-active-site catalyst displays a selectivity for formic acid consistently above 97% over a broad potential window (from −0.9 to −1.6 V <i>vs.</i> RHE). Even when fed with a low-concentration CO<sub>2</sub> stream (volume ratio from 50% down to 10%), the dual-active-site catalyst could display high activity and selectivity (>91%). In particular, the selectivity is still above 85% when the CO<sub>2</sub> volume ratio is as low as 5%. This work offers a feasible route for converting low-concentration CO<sub>2</sub> via a synergistic effect for dual-active-site 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 4","pages":"1620 - 1626"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716767","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

Lung-targeted polyzwitterionic lipid nanoparticles for effective treatment of lung inflammation

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2295-8

Wen Zhang, Jiaxin Li, Nan Wang, Muzi Li, Chen Peng, Xinyue Zhang, Guanghui Ouyang, Yan Li

{"title":"Lung-targeted polyzwitterionic lipid nanoparticles for effective treatment of lung inflammation","authors":"Wen Zhang, Jiaxin Li, Nan Wang, Muzi Li, Chen Peng, Xinyue Zhang, Guanghui Ouyang, Yan Li","doi":"10.1007/s11426-024-2295-8","DOIUrl":"10.1007/s11426-024-2295-8","url":null,"abstract":"<div><p>Lipid nanoparticles (LNPs) are non-viral nucleic acid delivery systems that show great potential in vaccine development and disease treatment. Although LNPs are particularly advantageous for <i>in vivo</i> delivery, the wide application of LNPs is impeded as their systemic delivery of nucleic acid drugs to extrahepatic tissues remains highly challenging. To address this issue, we developed lung-targeted polyzwitterionic LNPs with zwitterionic polymer poly(2-methyacryloyloxyethyl phosphorylcholine) (PMPC) modified 1,2-dimyristoyl-sn-glycerol lipid for the delivery of small interfering RNA (siRNA). Three libraries with 90 PMPC-LNPs@siRNA were established. The polyzwitterionic PMPC-LNPs had high siRNA encapsulation efficiency of about 90%. The findings revealed that polyzwitterionic PMPC-LNPs@siRNA absorbed protein corona with the main component of Vitronectin, mediating lung-targeted delivery of siRNA. With good cellular uptake and endo/lysosomal escape ability, <i>in vitro</i> and <i>in vivo</i> studies demonstrated that polyzwitterionic PMPC-LNPs with siRNA against tumor necrosis factor-α (TNF-α) could significantly down-regulate the TNF-α in mRNA and protein levels, and improved the pathological features of lung inflammation. Polyzwitterionic PMPC-LNPs@siRNA achieved safe and efficient treatment of lung inflammation. Therefore, this work offered a promising siRNA therapeutic approach for lung diseases.</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":"1107 - 1116"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475117","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

Near-infrared organic photosensitizers with aggregation-induced emission and switchable fluorescence for fungal infection therapy

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2325-2

Xinzhe Yang, Zixuan Huang, Keke Ding, Huili Yang, Lirong Wang, Qing Xia, Rong Hu, Guang Shi, Bingjia Xu, Anjun Qin

{"title":"Near-infrared organic photosensitizers with aggregation-induced emission and switchable fluorescence for fungal infection therapy","authors":"Xinzhe Yang, Zixuan Huang, Keke Ding, Huili Yang, Lirong Wang, Qing Xia, Rong Hu, Guang Shi, Bingjia Xu, Anjun Qin","doi":"10.1007/s11426-024-2325-2","DOIUrl":"10.1007/s11426-024-2325-2","url":null,"abstract":"<div><p>The development of near-infrared (NIR) photosensitizers with aggregation-induced emission (AIE) properties, switchable luminescence colors, and satisfactory photodynamic therapy (PDT) effects on the treatment of fungal infection is of great importance but very challenging. Herein, two ionic organic luminogens are constructed by employing diphenylamine, diphenylacrylonitrile/1,2-diphenylethene, and methylated quinoline cation as building blocks. It is found that the resulting compounds TCQF and TQF show apparent AIE properties and produce intense fluorescence with high photoluminescence quantum yields of up to 31.2% in the solid state. In the meantime, their emission colors can be switched between red and NIR and in the NIR region by mechanical force and solvent vapor, respectively, thereby enabling remarkable and reversible mechanochromism with emission variations of up to 104 nm. More excitingly, TCQF and TQF can efficiently generate ROS under the illumination of white light and show excellent antimicrobial activities and satisfactory PDT capabilities. Inspired by the unique anti-fungus properties, TCQF is employed as a biocompatible NIR photosensitizer for treating wound infection with <i>C. albicans</i>, and apparent PDT effects are achieved. This work provides a new direction for the development of multifunctional NIR materials with AIE properties.</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":"1426 - 1433"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716760","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

Encapsulating perovskite quantum dots into 3D COF for visible light-driven CO2 reduction

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2300-8

Xinxin Wang, Yucheng Jin, Xiya Yang, Qingyu Luan, Tianyu Wang, Dongdong Qi, Kang Wang, Jianzhuang Jiang

{"title":"Encapsulating perovskite quantum dots into 3D COF for visible light-driven CO2 reduction","authors":"Xinxin Wang, Yucheng Jin, Xiya Yang, Qingyu Luan, Tianyu Wang, Dongdong Qi, Kang Wang, Jianzhuang Jiang","doi":"10.1007/s11426-024-2300-8","DOIUrl":"10.1007/s11426-024-2300-8","url":null,"abstract":"<div><p>Lead halide perovskite quantum dots (LHP QDs) have been revealed to possess great potential in photocatalytic applications including CO<sub>2</sub> reduction, which however suffer from poor stability. Herein, a high crystalline hydrazine-linked three-dimensional (3D) covalent organic framework, USTB-17, was fabricated from the reaction between 12-connected building block and 4-connected 3,5,7-tetrakis(4-aldophenyl)-adamantane. Post-modification with Ni<sup>2+</sup> affords the metallic framework USTB-17(Ni) followed by sequential deposition of the CH<sub>3</sub>NH<sub>2</sub>PbI<sub>3</sub> (MAPbI<sub>3</sub>) perovskite QDs into its pores, generating the USTB-17(Ni)@MAPbI<sub>3</sub> composite. Powder X-ray diffraction analysis together with theoretical simulations and transmission electron microscopy discloses the crystalline nature of USTB-17, USTB-17(Ni), and USTB-17(Ni)@MAPbI<sub>3</sub> with an unprecedented non-interpenetrated <b>hpt</b> topology. The close contact of QDs inside the COF pores with the Ni catalytic site locating at the pore surface of COF allows a rapid transfer of the photogenerated electrons in QDs to the Ni catalytic sites, enhancing the photocatalytic activity for CO<sub>2</sub> reduction. This endows USTB-17(Ni)@MAPbI<sub>3</sub> with efficient photocatalysis performance for photocatalytic CO<sub>2</sub> reduction with CO generation rate of 365 µmol g<sup>−1</sup> h<sup>−1</sup> and CO selectivity up to 96% under visible-light irradiation, 7 times higher than that of USTB-17(Ni). After four cycles of reactions, the photocatalytic CO generation rate remains almost unchanged, demonstrating its excellent cycle stability.</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":"1478 - 1485"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716762","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

Tailor-made high elasticity and low-hysteresis hydrogels based on asymmetric H-bonding crosslinking for wearable applications

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2297-0

Xiaofang Shi, Nan Shi, Miaomiao Dang, Chengyu Ji, Yingjie Li, Peiyi Wu, Zhiguo Hu

{"title":"Tailor-made high elasticity and low-hysteresis hydrogels based on asymmetric H-bonding crosslinking for wearable applications","authors":"Xiaofang Shi, Nan Shi, Miaomiao Dang, Chengyu Ji, Yingjie Li, Peiyi Wu, Zhiguo Hu","doi":"10.1007/s11426-024-2297-0","DOIUrl":"10.1007/s11426-024-2297-0","url":null,"abstract":"<div><p>The conventional method of fabricating hydrogels constantly confronts the conflict between elasticity and toughness, limiting their repetitive application. Achieving the desired elasticity through a simple and low-cost approach is a significant challenge for hydrogels, particularly through rational molecular design. Here, low-hysteresis and high-toughness hydrogels are developed from the design of a new feature monomer, <i>N</i>-acryloylethylsemicarbazide (NACE). Based on a concept of “asymmetric H-bonding design”, the unique double and triple H-bonding of NACE can result in a novel asymmetric crosslinking polymer with alternating strong and weak H-bonding regions. The NACE is copolymerized with acrylamide (AM) to regulate the mechanical properties of hydrogel via H-bonding density. The P(NACE-AM) ionic hydrogels are obtained simply and rapidly via one-step photopolymerization without a chemical cross-linking agent. The P(NACE-AM) hydrogels combine superb mechanical elasticity and toughness, and excellent ionic conductivity, showing great potential as durable ionic conductive devices for wearable utilization.</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":"1117 - 1125"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475121","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

Impregnating photo-stable gold precursor onto uncalcined TS-1 to boost catalytic hydro-oxidation of propane

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2403-7

Zhihua Zhang, Erchuan Yang, Fan Liu, Kesheng Xu, Yuxia Zhong, Jinwei Sun, Shudong Shi, Xuezhi Duan, Xinggui Zhou

{"title":"Impregnating photo-stable gold precursor onto uncalcined TS-1 to boost catalytic hydro-oxidation of propane","authors":"Zhihua Zhang, Erchuan Yang, Fan Liu, Kesheng Xu, Yuxia Zhong, Jinwei Sun, Shudong Shi, Xuezhi Duan, Xinggui Zhou","doi":"10.1007/s11426-024-2403-7","DOIUrl":"10.1007/s11426-024-2403-7","url":null,"abstract":"<div><p>Immobilizing highly dispersed Au nanoparticles onto titanium silicalite-1 (TS-1) by a simple impregnation method under light is still a challenging task. In this work, a high photostable Au precursor protected by thiol ligands was firstly synthesized, and the as-prepared Au precursor displayed excellent stability under light for over 30 days, while the Au precursor without thiol ligands formed precipitates after just 2 h under light. Subsequently, the Au precursor protected by thiol ligands was immobilized on the external surface of uncalcined TS-1 (i.e., TS-1-B) by the incipient wetness impregnation method (IWI method) to prepare Au/TS-1-B catalyst. The activity of as-prepared Au/TS-1-B catalyst in the hydro-oxidation of propane to acetone was 1.4 times higher than that of the catalyst prepared by the deposition-precipitation urea method (DPU method). The structures of the Au/TS-1-B catalysts prepared by different methods were analyzed by multiple characterizations. Compared to the Au/TS-1-B catalyst prepared by the DPU method, the Au/TS-1-B catalyst synthesized by the IWI method exhibited a narrower size distribution of Au nanoparticles and had more small Au particles (<2 nm), which is the main reason for its superior activity. Additionally, the effects of gold loadings, reaction temperature and Si/Ti molar ratio on the catalytic performance of the Au/TS-1-B catalyst prepared by the IWI method were also investigated. In addition, the Au/TS-1-B catalyst prepared by the IWI method also exhibited excellent stability for over 140 h.</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":"1585 - 1596"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716684","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

Engineering N3C vacancies in hierarchical porous carbon nitride nanosheets for room temperature ultradeep photocatalytic aerobic oxidative desulfurization

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2306-1

Yina Nie, Weijie Yang, Xin Wang, Xiang Li, Lele Wei, Xiaolin Bai, Lin Liu, Feng Fu, Jun Wan

{"title":"Engineering N3C vacancies in hierarchical porous carbon nitride nanosheets for room temperature ultradeep photocatalytic aerobic oxidative desulfurization","authors":"Yina Nie, Weijie Yang, Xin Wang, Xiang Li, Lele Wei, Xiaolin Bai, Lin Liu, Feng Fu, Jun Wan","doi":"10.1007/s11426-024-2306-1","DOIUrl":"10.1007/s11426-024-2306-1","url":null,"abstract":"<div><p>The production of ultra-low sulfur clean fuels holds global significance for improving energy efficiency and reducing environmental pollution. Photocatalytic aerobic oxidative desulfurization (PODS) offers an attractive approach to efficiently remove refractory heterocyclic aromatic sulfur compounds under mild conditions. However, the sluggish charge dynamics, insufficient molecule activation, and slow mass transfer within photocatalysts restrict the overall desulfurization efficiency, hindering the widespread application of this technology. Herein, we developed a defective g-C<sub>3</sub>N<sub>4</sub> (M<sub>1</sub>U<sub>3</sub>CN) photocatalyst with bridged N<sub>3C</sub> vacancies and hierarchical porous structures to address these limitations. This catalyst not only demonstrates outstanding dibenzothiophene (DBT) removal efficiency of 99.6% for model oil with high conversion and selectivity but also achieves complete sulfur removal from gasoline as well as 96.7% sulfur removal for distilled diesel at room temperature, successfully achieving ultradeep aerobic oxidative desulfurization. The introduction of rich N<sub>3C</sub> vacancies and abundant micro-meso-macroporous distribution in M<sub>1</sub>U<sub>3</sub>CN enhances kinetic efficiencies by promoting charge carrier separation, mass transfer, and molecular activation simultaneously; resulting in exceptional PODS performance. This work provides a collaborative strategy to overcome kinetic challenges in aerobic oxidative desulfurization <i>via</i> defect and structural engineering of the catalyst.</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":"1608 - 1619"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716685","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

Physarum polycephalum-inspired adaptive optimization design of artificial microtubular networks

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2305-8

Si-Min Zeng, Di-Wei Zheng, Ting Pan, Xing-Lan Ding, Yun Zhang, Chi-Hui Yang, Si-Xue Cheng, Xian-Zheng Zhang

{"title":"Physarum polycephalum-inspired adaptive optimization design of artificial microtubular networks","authors":"Si-Min Zeng, Di-Wei Zheng, Ting Pan, Xing-Lan Ding, Yun Zhang, Chi-Hui Yang, Si-Xue Cheng, Xian-Zheng Zhang","doi":"10.1007/s11426-024-2305-8","DOIUrl":"10.1007/s11426-024-2305-8","url":null,"abstract":"<div><p>Natural biological microtubular networks have undergone adaptive evolutionary selection and may offer viable solutions to design challenges in artificial microtubular networks. The plasmodium of the slime mold <i>Physarum polycephalum</i> (<i>P. polycephalum</i>) extends continuously to form a protoplasmic microtubular network structure, directly connecting food sources. Computational simulations revealed that the formation of this adaptive <i>P. polycephalum</i> microtubular network could be captured by a mathematical algorithm. Inspired by the <i>P. polycephalum</i> microtubular networks, we propose an adaptive optimization design method for artificial microtubular networks. Specifically, we utilized hydrogels with biodegradable and tissue-adhesive properties to replicate the <i>P. polycephalum</i> microtubular networks <i>via</i> photomask. In Rhodamine B diffusion and glucose-catalyzed reaction experiments, we found that the <i>P. polycephalum</i> microtubular networks exhibited significantly enhanced efficiency compared to vascular and artificial networks. Furthermore, we demonstrated the potential for uric acid (UA) degradation of the hydrogels with a real <i>P. polycephalum</i> microtubular network loaded with urate oxidase (UOx) in a rodent model of hyperuricemia. And this network achieved more than double the effect of the artificial network. This underscores the potential of natural microtubular networks to replace artificial microtubular networks.</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":"1497 - 1510"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716763","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