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scalable preparation and direct visualization of cyclic polymers via self-folding cyclization technique

Science China Chemistry 2022年第12期65卷 2558-2566页

作者： Hualong Zhang Hao Zha Chao Liu Chunyan Hong CAS Key Laboratory of Soft Matter Chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefei230026China

Cyclic polymers exhibit distinct properties compared with their linear counterparts due to the lack of chain ends.However,the scalable synthesis of cyclic polymers remains a major challenge,especially for ring-closure method.Herein,we report a novel strategy for large-scale preparation of cyclic polymers,which relies on the prior self-folding of anthracene-telechelic amphiphilic random copolymers(poly((oligo(ethylene glycol)acrylate)-co-(dodecyl acrylate)),P(OEGA-co-DDA))into single-chain polymeric nanoparticles(SCPNs)in water.Subsequent ultraviolet(UV)-induced cyclization occurs in the hydrophobic nano-domain.The formation of SCPNs leads to a shortened distance between the end groups of the linear precursors and spatially separated cyclization loci,and significantly enhances the efficiency of UV-induced cyclization.This self-folding technique permits access to the synthesis of cyclic polymers not only with high molecular weights(M_(n)>10^(5) g/mol),but also in a decent scale(40 g/L),breaking through the limitations of ring-closure method.Furthermore,the dense pendants of the copolymers can magnify the macromolecules by increasing the mass density along the backbones,thus making the polymers more readily detectable by the microscopy.The transmission electron microscopy(TEM)and atomic force microscopy(AFM)images allow us to observe the topological structures directly and provide crucial evidence to confirm the cyclization.

关键词： cyclic polymer scalable preparation direct visualization self-folding cyclization technique

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Hydrogen-assisted scalable preparation of ultrathin Pt shells onto surfactant-free and uniform Pd nanoparticles for highly efficient oxygen reduction reaction in practical fuel cells

引用

Nano Research 2022年第3期15卷 1892-1900页

作者： Liuxuan Luo Cehuang Fu Aiming Wu Zechao Zhuang Fengjuan Zhu Fangling Jiang Shuiyun Shen Xiyang Cai Qi Kang Zhifeng Zheng Chenyi Hu Jiewei Yin Guofeng Xia Junliang Zhang Institute of Fuel Cells Key Laboratory for Power Machinery and Engineering of MOESchool of Mechanical EngineeringShanghai Jiao Tong UniversityShanghai 200240China Department of Chemistry Tsinghua UniversityBeijing 100084China The State Key Lab of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 201899China Department of Polymer Science and Engineering Shanghai Key Laboratory of Electrical Insulation and Thermal AgeingShanghai Jiao Tong UniversityShanghai 200240China

Concentrating active Pt atoms in the outer layers of electrocatalysts is a very effective approach to greatly reduce the Pt loading without compromising the electrocatalytic performance and the total electrochemically active surface area(ECSA)for the oxygen reduction reaction(ORR)in hydrogen-based proton-exchange membrane fuel cells.Accordingly,a facile,low-cost,and hydrogen-assisted two-step method is developed in this work,to massively prepare carbon-supported uniform,small-sized,and surfactant-free Pd nanoparticles(NPs)with ultrathin~3-atomic-layer Pt shells(Pd@Pt_(3L) NPs/C).Comprehensive physicochemical characterizations,electrochemical analyses,fuel cell tests,and density functional theory calculations reveal that,benefiting from the ultrathin Pt-shell nanostructure as well as the resulting ligand and geometric effects,Pd@Pt_(3L) NPs/C exhibits not only significantly enhanced ECSA,electrocatalytic activity,and noble-metal(NM)utilization compared to commercial Pt/C,showing 81.24 m^(2)/gPt,0.710 mA/cm^(2),and 352/577 mA/mgNM/Pt in ECSA,area-,and NM-/Pt-mass-specific activity,respectively;but also a much better electrochemical stability during the 10,000-cycle accelerated degradation test.More importantly,the corresponding 25-cm^(2) H2-air/O_(2) fuel cell with the low cathodic Pt loading of~0.152 mgPt/cm^(2)geo achieves the high power density of 0.962/1.261 W/cm^(2)geo at the current density of only 1,600 mA/cm^(2)geo,which is much higher than that for the commercial Pt/C.This work not only develops a high-performance and practical Pt-based ORR electrocatalyst,but also provides a scalable preparation method for fabricating the ultrathin Pt-shell nanostructure,which can be further expanded to other metal shells for other energy-conversion applications.

关键词： palladium platinum oxygen reduction reaction core@shell nanostructure scalable preparation proton-exchange membrane fuel cell

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