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A review on plasmonic enhancement of activity and selectivity in electrocatalytic CO_(2)reduction

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Frontiers in Energy 2024年第4期18卷 399-417页

作者： Jing XUE Zhenlin CHEN Yuchao ZHANG Jincai ZHAO key laboratory of photochemistry Beijing National Laboratory for Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of chinese academy of sciences Beijing 100049China

Utilizing plasmonic effects to assist electrochemical reactions exhibits a huge potential in tuning the reaction activities and product selectivity,which is most appealing especially in chemical reactions with multiple products,such as CO_(2)reduction reaction(CO_(2)RR).However,a comprehensive review of the development and the underlying mechanisms in plasmon-assisted electrocatalytic CO_(2)RR remains few and far ***,the fundamentals of localized surface plasmonic resonance(LSPR)excitation and the properties of typical plasmonic metals(including Au,Ag,and Cu)are ***,the potential mechanisms of plasmonic effects(such as hot carrier effects and photothermal effects)on the reaction performance in the field of plasmon-assisted electrocatalytic CO_(2)RR are summarized,which provides directions for the future development of this *** is concluded that plasmonic catalysts exhibit potential capabilities in enhancing CO_(2)RR while more in situ techniques are essential to further clarify the inner mechanisms.

关键词： localized surface plasmonic resonance(LSPR)effect plasmonic metals CO_(2)reduction reaction(CO_(2)RR) hot carrier effect photothermal effect

Triplet-triplet annihilation upconversion materials as electrophoretic inks

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chinese Chemical Letters 2024年第3期35卷 439-442页

作者： Qiaoyu Zhang Guiwen Luo Jinping Chen Tianjun Yu Rui Hu Guoqiang Yang Yi Zeng Yi Li key laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China key laboratory of photochemistry Institute of ChemistryChinese Academy of SciencesBeijing 100190China University of chinese academy of sciences Beijing 100049China

Luminescent materials that can be reversibly switched by electric field stimulation are attractive since the potential application for optoelectronic *** we report a triplet-triplet annihilation upconversion(TTA-UC)system with electrophoretic response which is developed as the electrophoretic *** TTA-UC system consists of an ionic derivative of 9,10-diphenyl anthracene(DPA)as the annihilator and Pt(II)octaethylporphyrin(PtOEP)as the *** applying an electric field,migration and enrichment of positively charged DPA derivatives towards the cathode results in a 20%enhancement of TTA-UC.A quasi-solid film for electrically writing is made using the electrophoretic TTA system as the ink and a platinum electrode as a *** prototype of TTA-UC ink demonstrates unique luminescence functions upon electrically writing and erasing,providing a promising strategy to develop electronic devices for display,information storage and encryption.

关键词： Triplet-triplet annihilation Photon upconversion Electrophoresis Electrophoretic ink Luminescence display

Nitrogen-doping boosts *CO utilization and H2O activation on copper for improving CO2 reduction to C2+ products

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Green Energy & Environment 2024年第9期9卷 1459-1465页

作者： Yisen Yang Zhonghao Tan Jianling Zhang Jie Yang Renjie Zhang Sha Wang Yi Song Zhuizhui Su Beijing National laboratory for Molecular sciences CAS Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Center for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences School of Chemical sciences University of Chinese Academy of Sciences key laboratory of photochemistry CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences

To improve the electrocatalytic transformation of carbon dioxide （CO2） to multi-carbon (C2+) products is of great *** we developed a nitrogen-doped Cu catalyst,by which the maximum C2+Faradaic efficiency can reach 72.7%in flow-cell system,with the partial current density reaching 0.62 A *** in situ Raman spectra demonstrate that the *CO adsorption can be strengthened on such a N-doped Cu catalyst,thus promoting the*CO utilization in the subsequent C–C coupling ***,the water activation can be well enhanced by N doping on Cu *** to the synergistic effects,the selectivity and activity for C2+products over the N-deoped Cu catalyst are much improved.

关键词： Electrocatalytic CO 2 reduction reaction Copper catalyst Doping Multi-carbon products In situ Raman measurement

Modularized viromimetic polymer nanoparticle vaccines(VPNVaxs) to elicit durable and effective humoral immune responses

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National Science Review 2024年第3期11卷 200-214页

作者： Zichao Huang Xinyu Zhuang Liping Liu Jiayu Zhao Sheng Ma Xinghui Si Zhenyi Zhu Fan Wu Ningyi Jin Mingyao Tian Wantong Song Xuesi Chen key laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of Sciences School of Applied chemistry and Engineering University of Science and Technology of China Changchun Veterinary Research institute Chinese Academy of Agricultural Sciences Jilin Biomedical Polymers Engineering laboratory State key laboratory of Polymer Physics and chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences

Virus-like particle(VLP) vaccines had shown great potential during the COVID-19 pandemic, and was thought to be the next generation of antiviral vaccine technology due to viromimetic structures. However,the time-consuming and complicated processes in establishing a current recombinant-protein–based VLP vaccine has limited its quick launch to the out-bursting pandemic. To simplify and optimize VLP vaccine design, we herein report a kind of viromimetic polymer nanoparticle vaccine(VPNVax), with subunit receptor-binding domain(RBD) proteins conjugated to the surface of polyethylene glycol-b-polylactic acid(PEG-b-PLA) nanoparticles for vaccination against SARS-CoV-2. The preparation of VPNVax based on synthetic polymer particle and chemical post-conjugation makes it possible to rapidly replace the antigens and construct matched vaccines at the emergence of different viruses. Using this modular preparation system, we identified that VPNVax with surface protein coverage of 20%–25% had the best immunostimulatory activity, which could keep high levels of specific antibody titers over 5 months and induce virus neutralizing activity when combined with an aluminum adjuvant. Moreover, the polymer nano-vectors could be armed with more immune-adjuvant functions by loading immunostimulant agents or chemical chirality design. This VPNVax platform provides a novel kind of rapidly producing and efficient vaccine against different variants of SARS-CoV-2 as well as other viral pandemics.

关键词： vaccine polymer nanomaterials SARS-CoV-2

The critical role of energetic fluctuations in charge separation for efficient molecular doping of organic semiconductors

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Science China chemistry 2024年第11期67卷 3675-3680页

作者： Yan Zeng Guangchao Han Yuanping Yi Beijing National laboratory for Molecular sciences CAS Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences University of chinese academy of sciences

Molecular doping is essential to improve the electrical conductivity of organic semiconductors for high-performance organic electronic devices. However, the doping efficiency is influenced by several factors, such as the energy levels, energetic fluctuations, dielectric properties, and molecular packing structures of the doped films, and the underlying mechanisms for highefficiency doping are still unclear. Here, through multi-level theoretical simulations on a series of fullerene derivatives, we identify that the energetic fluctuations can play a decisive role in activating charge separation for molecular doping. In particular,the doping efficiency appears to be exponentially increased with the fluctuation of charge polarization energies. Therefore,although the charge mobility is somewhat decreased, the experimental electrical conductivity is improved with the increased energetic fluctuation. Moreover, it has been found that polarization energy fluctuation can be effectively enhanced by simply introducing side chains with greater flexibility into organic semiconductors. This article paves the way towards high-efficiency molecular doping of organic semiconductors.

关键词： doping efficiency polarization energies energetic fluctuations organic semiconductors

Furfural residues derived nitrogen-sulfur co-doped sheet-like carbon: An excellent electrode for dual carbon lithium-ion capacitors

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Green Energy & Environment 2024年第9期9卷 1427-1439页

作者： Xiaoying Guo Yan Qiao Zonglin Yi Christian Marcus Pedersen Yingxiong Wang Xiaodong Tian Peide Han College of Materials Science and Engineering Taiyuan University of Technology State key laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences University of chinese academy of sciences CAS key laboratory of Carbon Materials Institute of Coal Chemistry Chinese Academy of Sciences Department of chemistry University of Copenhagen Universitetsparken 5 College of chemistry Taiyuan University of Technology

The state-of-the-art lithium-ion capacitors （LICs）,consisting of high-capacity battery-type anode and high-rate capacitor-type cathode,can deliver high energy density and large power density when comparing with traditional supercapacitors and lithium-ion batteries,***,the ion kinetics mismatch between cathode and anode leads to unsatisfied cycling lifetime and anode *** efforts have been devoted to solving the abovementioned *** promising strategy is altering high conductive hard carbon anode with excellent structural stability to match with activated carbon cathode,assembling dual-carbon *** this contribution,one-pot in-situ expansion and heteroatom doping strategy was adopted to prepare sheet-like hard carbon,while activated carbon was obtained involving *** persulfate was used as expanding and doping agent *** furfural residues （FR） were served as carbon *** resulting hard carbon （FRNS-HC） and activated carbon （FRNS-AC）show excellent electrochemical performance as negative and positive electrodes in a lithium-ion battery （LIB）.To be specific,374.2 m Ah g-1and 123.1 m Ah g-1can be achieved at 0.1 A g-1and 5 A g-1when FRNS-HC was tested as *** combined with a highly porous carbon cathode (SBET=2961 m2g-1) synthesized from the same precursor,the LIC showed high specific energy of147.67 Wh kg-1at approximately 199.93 W kg-1,and outstanding cycling life with negligible capacitance fading over 1000 *** study could lead the way for the development of heteroatom-doped porous carbon nanomaterials applied to Li-based energy storage applications.

关键词： Furfural residue Ammonium persulfate Sheet-like carbon Lithium-ion capacitors Hard carbon

Sustainable, thermoplastic and hydrophobic coating from natural cellulose and cinnamon to fabricate eco-friendly catering packaging

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Green Energy & Environment 2024年第5期9卷 927-936页

作者： Rumeng Xu Chunchun Yin Jingxuan You Jinming Zhang Qinyong Mi Jin Wu Jun Zhang CAS key laboratory of Engineering Plastics Institute of ChemistryChinese Academy of Sciences(CAS)Beijing100190China University of chinese academy of sciences Beijing100049China

Non-degradable polymers cause serious environmental pollution problem,such as the widely-used while unrecyclable coatings which signiﬁcantly affect the overall degradation performance of *** is imperative and attractive to develop biodegradable functional ***,we proposed a novel strategy to successfully prepare biodegradable,thermoplastic and hydrophobic coatings with high transparence and biosafety by weakening the interchain interactions between cellulose *** natural cellulose and cinnamic acid were as raw *** reducing the degree of polymerization(DP)of cellulose and regulating the degree of substitution(DS)of cinnamate moiety,the obtained cellulose cinnamate(CC)exhibited not only the thermalﬂow behavior but also good biodegradability,which solves the conﬂict between the thermoplasticity and biodegradability in cellulose-based *** glass transition temperature(T_(g))and thermalﬂow temperature(T_(f))of the CC could be adjusted in a range of 150–200℃ and 180–210℃,*** CC with DS<1.2 and DP≤100 degraded more than 60%after an enzyme treatment for 7 days,and degraded more than 80%after a composting treatment for 42 ***,CC had no toxicity to human epidermal cells even at a high concentration(0.5 mg mL^(-1)).In addition,CC could be easily fabricated into multifunctional coating with high hydrophobicity,thermal adhesion and high ***,after combining with cellophane and paperboard,CC coating with low DP and DS could be used to prepare fully-biodegradable heat-sealing packaging,art paper,paper cups,paper straws and food packaging boxes.

关键词： Thermoplastic coating Bio-degradable adhesive Natural products Cellulose Eco-friendly packaging

Control of aluminum distribution in ZSM-5 zeolite for enhancement of its catalytic performance for propane aromatization

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Frontiers of Chemical Science and Engineering 2024年第8期18卷 15-24页

作者： Zhao Ma Dezhi Shi Sen Wang Mei Dong Weibin Fan State key laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China University of chinese academy of sciences Beijing 100049China

Regulation of aluminum distribution in zeolite framework is an effective method for improving its catalytic performance for propane ***,we found that recrystallization and post-realuminization of ZSM-5 cannot only create hollow structures to enhance the diffusion ability,but also adjust the content and position of paired aluminum species in its *** characterizations results confirmed that increase of paired aluminum content and inducement of more aluminum atoms sited in the intersection cavity are beneficial to the formation of aromatic products in propane *** a result,the hollow-structured ZSM-5 zeolite with more paired aluminum(H-200-hollow)showed higher propane conversion and aromatics selectivity than other samples at the same *** catalytic performance of H-200-hollow can be further improved by ion-exchanging with a small amount of Ga(III)*** propane conversion and aromatics selectivity of Ga-200-hollow reached as high as 95%and 70%,respectively,at 540°C and 1 atm.

关键词： propane aromatization zeolite aluminum distribution recrystallization and post-realuminization

Degradation mechanisms and stabilization strategies of ruthenium-based catalysts for OER in the proton exchange membrane water electrolyzer

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Progress in Natural Science:Materials International 2024年第1期34卷 207-222页

作者： Ming Yang Hongxiang Wu Zhaoping Shi Yibo Wang Jiahao Yang Jing Ni Pengbo Wang Yuqing Cheng Ziang Wang Meiling Xiao Changpeng Liu Wei Xing laboratory of Advanced Power Sources Changchun Institute of Applied Chemistry Chinese Academy of Sciences School of Applied chemistry and Engineering University of Science and Technology of China Jilin Province key laboratory of Low Carbon Chemical Power Sources State key laboratory of Electroanalytical chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences

Designing economical oxygen evolution reaction(OER) electrocatalysts with high activity and long-term stability is essential to promote the scale-up applications of proton exchange membrane water electrolyzer(PEMWE) for hydrogen production. Ruthenium(Ru)-based materials with high intrinsic activity are hailed as the most promising catalysts, but still infeasible for practical application considering their long unresolved poor stability(only dozens of lifespan). Thus, tremendous efforts have been devoted to uncovering the degradation mechanisms and developing stabilization strategies for the Ru-based catalysts. In this review, starting from summarizing the fundamental understanding of deactivation mechanisms, a picture of the stability issue of Ru-based catalysts is proposed, which is followed by a detailed discussion on the recently developed strategies and progress made on enhancing durability. Finally, insights on the prospects for the future development of stable and practical Rubased OER catalysts are provided.

关键词： OER Ru-based catalysts PEMWE Degradation mechanisms Stabilization strategies