Science China Chemistry最新文献_第8页

Tetraphenylethylene dicycle helicates: circularly polarized luminescence and chiral recognition based on emission wavelength change 四苯基乙烯二环螺旋体：圆偏振发光和基于发射波长变化的手性识别

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-09 DOI: 10.1007/s11426-024-2145-y

Zhi-Rong Xu, Miao-Li Gao, Ming Hu, Wei Yu, Yan-Song Zheng

{"title":"Tetraphenylethylene dicycle helicates: circularly polarized luminescence and chiral recognition based on emission wavelength change","authors":"Zhi-Rong Xu, Miao-Li Gao, Ming Hu, Wei Yu, Yan-Song Zheng","doi":"10.1007/s11426-024-2145-y","DOIUrl":"10.1007/s11426-024-2145-y","url":null,"abstract":"<div><p>Chiral tetraphenylethylene (TPE) dicycle tetraaldehyde and TPE dicycle tetraacids bearing optically pure groups on the cycles were designed and synthesized. Due to the propeller-like conformation immobilization of TPE unit, this new class of TPE dicycle was resolved into <i>M</i>- and <i>P</i>-enantiomers, which could emit strong circular polarized luminescence (CPL). Interestingly, these TPE helicates displayed exceptional ability of molecule recognition. While the TPE dicycle tetraaldehyde could detect the microscale water in anhydrous tetrahydrofuran, the chiral TPE dicycle tetraacid could display different fluorescent color after interacting with two enantiomers of a wide variety of chiral amines including monoamines, diamines, and aminols, which could be applied to chiral recognition of these chiral amines. Furthermore, the emission wavelength of TPE dicycle tetraacid was found to change linearly with the enantiomer purity of chiral amine from enantiomer excess (<i>ee</i>) percent −100% to +100%, for the first time showing the potential for quantitative chiral analysis of chiral amines based on emission wavelength change. The emission wavelength was affected less by environmental factors than fluorescence intensity, which would enable the chiral analysis based on wavelength change with higher accuracy and repeatability.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 11","pages":"3817 - 3824"},"PeriodicalIF":10.4,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197162","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

Reconstructed parallel sites enhance the reactive oxygen tolerance of non-noble metal catalyst for durable proton exchange membrane fuel cells 重构平行位点增强了非贵金属催化剂对活性氧的耐受性，从而实现持久的质子交换膜燃料电池

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-09 DOI: 10.1007/s11426-024-2067-0

Wenjie Wang, Hui Ding, Minghao Wang, Han Cheng, Xiang Shi, Lin Wang, Chun Wang, Wangsheng Chu, Yi Xie, Changzheng Wu

{"title":"Reconstructed parallel sites enhance the reactive oxygen tolerance of non-noble metal catalyst for durable proton exchange membrane fuel cells","authors":"Wenjie Wang, Hui Ding, Minghao Wang, Han Cheng, Xiang Shi, Lin Wang, Chun Wang, Wangsheng Chu, Yi Xie, Changzheng Wu","doi":"10.1007/s11426-024-2067-0","DOIUrl":"10.1007/s11426-024-2067-0","url":null,"abstract":"<div><p>The establishment of reactive oxygen species (ROS) elimination sites in iron-nitrogen-carbon (Fe-N-C) electrocatalysts to achieve durable proton-exchange membrane fuel cells (PEMFCs) performance has attracted broad interest. However, realizing ROS removal efficiency and oxygen reduction reaction (ORR) activity within a single system represents a significant challenge to date. Herein, we demonstrate uniform ROS elimination sites and ORR centers through an electrochemical reconstruction method on the parallel sites of Fe@CeNC electrocatalyst for durable PEMFC. During the reconstruction process, the Fe sites can retain their original configuration. Meanwhile, the pristine Ce clusters will evolve into more efficient, highly dispersed sites. Furthermore, the reconstructed Fe and Ce sites exhibit favorable energy barriers for the ORR and ROS elimination pathways, respectively, thereby maintaining ORR activity and achieving high ROS tolerance. Consequently, the PEMFC assembled with our catalyst shows only a 2% decay in power density after the accelerated durability test. We anticipate that this parallel structure design will provide new insight into the development of more durable electrocatalysts for PEMFCs.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 11","pages":"3739 - 3748"},"PeriodicalIF":10.4,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197153","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

Active sites and reaction mechanisms of COx hydrogenation on zinc-based mixed oxide catalysts 锌基混合氧化物催化剂上 COx 加氢的活性位点和反应机理

IF 9.445 1区化学

Science China Chemistry Pub Date : 2024-09-09 DOI: 10.1007/s11426-024-2212-0

Zhuo-Yan Yao, Sicong Ma, Zhi-Pan Liu

引用次数: 0

Electrocatalysis for sustainable nitrogen management: materials innovation for sensing, removal and upcycling technologies 用于可持续氮管理的电催化技术：用于传感、去除和再循环技术的材料创新

IF 9.445 1区化学

Science China Chemistry Pub Date : 2024-09-09 DOI: 10.1007/s11426-024-2286-7

Mei Yi, Hongmei Li, Minghao Xie, Panpan Li, Zhaoyu Jin, Guihua Yu

{"title":"Electrocatalysis for sustainable nitrogen management: materials innovation for sensing, removal and upcycling technologies","authors":"Mei Yi, Hongmei Li, Minghao Xie, Panpan Li, Zhaoyu Jin, Guihua Yu","doi":"10.1007/s11426-024-2286-7","DOIUrl":"https://doi.org/10.1007/s11426-024-2286-7","url":null,"abstract":"<p>The global nitrogen cycle holds immense importance due to its crucial role in supporting life, supplying vital nutrients for plant growth, preserving environmental balance, and enabling the proper functioning of ecosystems. However, human activities frequently disrupt this cycle, leading to the accumulation of nitrates and nitrites in water bodies. This accumulation causes environmental pollution and health risks. Traditional methods for treating nitrogen pollution, including biological, physical, and chemical approaches, have inherent limitations. In recent years, electrocatalysis has emerged as a promising and sustainable approach for nitrogen management. This technology offers superior efficiency, high selectivity, and environmental friendliness. It not only enables accurate detection of nitrogen pollutants in the environment but also facilitates their conversion into harmless nitrogen gas. Moreover, recent advancements have focused on the upcycling of nitrogen pollutants into valuable compounds, such as ammonia and urea. In this comprehensive review, we showcase the applications of electrocatalysis in sustainable nitrogen management. Specifically, we highlight its use in the sensing, removal, and upcycling of major nitrogen pollutants, including nitrate (NO<sub>3</sub><sup>−</sup>), nitrite (NO<sub>2</sub><sup>−</sup>), and nitric oxide (NO). We discuss the use of catalysts, such as Pd alloys, Cu-based, and Fe-based materials, in electrochemical sensing and catalysis. Additionally, we explore recent advancements in the conversion of nitrogen pollutants into valuable compounds like ammonia and urea. The review also addresses current challenges and future opportunities in the field, including innovations in sensor and catalyst design, as well as large-scale treatment strategies. We anticipate that these perspectives will provide profound insights for effective nitrogen pollution control and sustainable utilization of nitrogen resources.</p>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"11 1","pages":""},"PeriodicalIF":9.445,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197155","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

Horizontal oscillation processed large MXene with Low Ti–Ti coordination for fast sodium storage 水平振荡加工的低钛-钛配位大型 MXene，用于快速储钠

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-09 DOI: 10.1007/s11426-024-2063-5

Hang Wang, Xingwu Zhai, Yujian Xia, Zhixin Sun, Tianchen Wei, Guangyu Chen, Yuhuan Li, Xinfeng Tang, Liang Wu, Zhaodi Fan, Hongjun Zhang, Bangjiao Ye, Xueyuan Leng, Min Zhou

{"title":"Horizontal oscillation processed large MXene with Low Ti–Ti coordination for fast sodium storage","authors":"Hang Wang, Xingwu Zhai, Yujian Xia, Zhixin Sun, Tianchen Wei, Guangyu Chen, Yuhuan Li, Xinfeng Tang, Liang Wu, Zhaodi Fan, Hongjun Zhang, Bangjiao Ye, Xueyuan Leng, Min Zhou","doi":"10.1007/s11426-024-2063-5","DOIUrl":"10.1007/s11426-024-2063-5","url":null,"abstract":"<div><p>MXene stands out as a rising family of transition metal carbides/nitrides with exceptional size-dependent properties and versatile potential applications. However, the realization of large MXene with a controllable surface at atomic level remains challenging to keep the balance among the conductivity, stability and activity. Herein, the horizontal oscillation-induced delamination (HOD) strategy is proposed to acquire Ti<sub>3</sub>C<sub>2</sub> flakes with large size and low Ti–Ti coordination (HO-Ti<sub>3</sub>C<sub>2</sub>). The average size of the as-obtained flakes can reach 6.48 µm to keep the overall conductive skeleton and merits from large size. Simultaneously, metal atoms at surface can be partially removed due to the enhanced local vibrational turbulence during the reciprocating horizontal oscillation process. Such MXenes with clear and unique surface states exhibit high potentials in ion adsorption together with satisfied electric conductivity and stability. As proof of concept, HO-Ti<sub>3</sub>C<sub>2</sub> anode exhibits remarkable rate capability and long-term stability during sodium storage. A capacity of 100.5 mAh g<sup>−1</sup> with a long-life cycle (4,500 cycles) at a high rate of 1.0 A g<sup>−1</sup> originates from the increased s-d interaction between Na and Ti. Therefore, the HOD strategy provides a controllable surface design to promote the clear criteria into size-dependent research on MXene.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 11","pages":"3729 - 3738"},"PeriodicalIF":10.4,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197152","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

Chiral helically grooved gold nanoarrows for concurrently enhancing oxygen and hydrogen evolution from electrochemical water splitting 手性螺旋槽金纳米箭，用于同时提高电化学水分解的氧气和氢气进化能力

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-06 DOI: 10.1007/s11426-024-2136-1

Lufei Huang, Tao Wang, Ying Li, Ping Wang, Rui Tian, Baowen Zhou, Lin Yao

{"title":"Chiral helically grooved gold nanoarrows for concurrently enhancing oxygen and hydrogen evolution from electrochemical water splitting","authors":"Lufei Huang, Tao Wang, Ying Li, Ping Wang, Rui Tian, Baowen Zhou, Lin Yao","doi":"10.1007/s11426-024-2136-1","DOIUrl":"10.1007/s11426-024-2136-1","url":null,"abstract":"<div><p>Electrocatalytic water splitting shows a tremendous promise for storing green and intermittent electricity into storable fuels, paving a sustainable way toward carbon neutrality. The exploration of a bifunctional electrocatalyst for simultaneously enhancing oxygen evolution reaction and hydrogen evolution reaction is at the core yet remains a grand challenge, especially operated in the same electrolyte. In this work, mesoscale gold nanoarrows with special chiral morphology are synthesized for electrocatalytic water splitting. In the same electrolyte of 1 M KOH aqueous solution, the as-designed chiral R-/L-helically grooved gold nanoarrows (R-/L-heliGNAs) demonstrated significantly enhanced performance in both hydrogen evolution reaction and oxygen evolution reaction with overpotentials of 186 and 355 mV at 10 mA cm<sup>−2</sup>, respectively, compared to the achiral counterpart. For oxygen evolution reaction, the performance is even comparable to commercial notable metal catalysts, i.e., RuO<sub>2</sub>, of which the overpotential is 310 mV under the same measured conditions. The spin-polarized conductive atomic force microscope (c-AFM), finite-difference time-domain simulation, in combination with electrochemical investigations, show that the chirality of R-/L-heliGNAs makes a substantial contribution toward the remarkable performance by enhanced electric field distribution for hydrogen evolution reaction and by tuning the spin states of the electrons for oxygen evolution reaction. This study presents an encouraging strategy for simultaneously promoting hydrogen evolution reaction and oxygen evolution reaction that operated in the same electrolyte by imparting chirality toward a mesoscale inorganic electrocatalyst, showing a grand promise for opening up a new way for electrocatalytic water splitting toward green hydrogen.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 11","pages":"3767 - 3776"},"PeriodicalIF":10.4,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197164","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

Controllable selective anchoring of subnanometric Ru clusters or single-atoms/clusters on tungsten nitride for the hydrogen oxidation 在氮化钨上可控地选择性锚定亚纳米级 Ru 簇或单原子/簇，以实现氢氧化

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-06 DOI: 10.1007/s11426-024-2068-1

Qijiao Sun, Chuanqiang Wu, Yiqiang Sun, Yuan Shen, Lei Zhao, Xiaodong Yang, Li Yang, Yunxiang Lin, Keke Mao, Kun Xu

{"title":"Controllable selective anchoring of subnanometric Ru clusters or single-atoms/clusters on tungsten nitride for the hydrogen oxidation","authors":"Qijiao Sun, Chuanqiang Wu, Yiqiang Sun, Yuan Shen, Lei Zhao, Xiaodong Yang, Li Yang, Yunxiang Lin, Keke Mao, Kun Xu","doi":"10.1007/s11426-024-2068-1","DOIUrl":"10.1007/s11426-024-2068-1","url":null,"abstract":"<div><p>The impregnation method in the preparation of metal cluster catalysts typically inadvertently introduces single atoms (SAs) into the substrate. However, the question of whether the introduction of SAs will further improve the catalytic activity of cluster systems for specific reactions such as the hydrogen oxidation reaction (HOR) remains unraveled. Herein, we demonstrate Ru clusters anchored on WN nanowires (Ru<sub>C</sub>/WN) show a higher alkaline HOR catalytic activity in comparison with Ru SAs and nanoclusters (NCs)-coupled catalyst anchored on WN nanowires system (Ru<sub>C,S</sub>/WN). Notably, the Ru<sub>C</sub>/WN exhibits superb intrinsic catalytic activity with a mass-normalized exchange current density of 890 mA mg<sup>−1</sup><sub>PGM</sub>, which is among the top level of well developed Ru-based HOR catalysts. Both theoretical simulation and experimental investigation suggest that Ru<sub>C</sub>/WN owns an optimized H<sup>*</sup> and OH<sup>*</sup> reaction intermediates for the alkaline HOR, therefore resulting in the excellent intrinsic HOR catalytic performance.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 11","pages":"3749 - 3756"},"PeriodicalIF":10.4,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197165","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

Recent development in electrode design for wide-temperature supercapacitors 宽温超级电容器电极设计的最新进展

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-06 DOI: 10.1007/s11426-024-2149-x

Jianhong Liu, Qiang Zhou, Yuxiao Lin, Xinsheng Zhao, Guangmin Zhou, Xiaoxiao Li

{"title":"Recent development in electrode design for wide-temperature supercapacitors","authors":"Jianhong Liu, Qiang Zhou, Yuxiao Lin, Xinsheng Zhao, Guangmin Zhou, Xiaoxiao Li","doi":"10.1007/s11426-024-2149-x","DOIUrl":"10.1007/s11426-024-2149-x","url":null,"abstract":"<div><p>An ever-increasing market demand has stimulated the soaring enthusiasm of researchers to develop wide-temperature super-capacitors (SCs). The active electrode is one of the most important parts of SC, which is directly related to the energy density, power transmission and long-term cyclability of the device in the wide-temperature environment. Compared with the SC electrodes aimed for room-temperature application, the SC electrodes for operating at wide-temperature scene often face greater challenges. In this review, the main challenges of SC electrodes under various temperature conditions, including low, high and cross-fade temperatures, are summarized. The relevant performance decay and failure mechanisms of wide-temperature SC electrodes are analyzed. In addition, this review deals with the recent studies and developments in robust wide-temperature SC electrodes with respect to the rational design of electrode structures and the exploitation of advanced active materials. Finally, the future directions for exploring reliable wide-temperature SCs are also proposed.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 1","pages":"96 - 117"},"PeriodicalIF":10.4,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142225141","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}

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Coordination-driven self-assembly of a molecular 818 knot and molecular borromean rings 分子 818 结和分子硼罗环的配位驱动自组装

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-06 DOI: 10.1007/s11426-024-2064-7

Xiang Gao, Dong Liu, Hai-Ning Zhang, Guo-Xin Jin

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Manufacture the conducting polymer with light

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-06 DOI: 10.1007/s11426-024-2239-4

Yang Li, Tianyu Li, Yan Ji, Baoguang Liu

引用次数: 0