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Electrocatalysis for sustainable nitrogen management: materials innovation for sensing, removal and upcycling technologies

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science China Chemistry 2025年第6期68卷 2322-2342页

作者： Mei Yi Hongmei Li Minghao Xie Panpan Li Zhaoyu Jin Guihua Yu Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China College of Materials Science and Engineering and College of Chemistry Sichuan University Materials Science and Engineering Program and Walker Department of Mechanical Engineering The University of Texas at Austin

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 *** 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（NO3-）, nitrite（NO2-）, 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.

关键词： electrocatalysis electrochemical sensor nitrogen removal ammonia electrosynthesis C–N coupling

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Tailored architecture of composite electrolyte for all-solid-state sodium batteries with superior rate performance and cycle life

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Nano Research 2024年第5期17卷 4171-4180页

作者： Xiang Guan Zhenhua Jian Xingan Liao Wenchao Liao Yanfei Huang Dazhu Chen Robert K.Y.Li Chen Liu Shenzhen Key Laboratory of Polymer Science and Technology Guangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhen 518055China Department of Materials Science and Engineering City University of Hong KongHong KongChina

Seeking for composite electrolytes reinforced all-solid-state sodium ion batteries with superior long lifespan and rate performance remains a great ***,a unique strategy to tailor the architecture of composite electrolyte via inserting polymer chains into a small quantity of sulfate sodium grafted C_(48)0H_(28)O_(32)Zr_(6)(UIOSNa)is *** intimate contact between polymer segments and UIOSNa with limited pore size facilitates the anion immobilization of sodium salts and reduction of polymer crystallinity,thereby providing rapid ion conduction and reducing the adverse effect caused by the immigration of *** tNa+grafting of-SO_(3)Na groups on fillers allows the free movement of more sodium ions to further improve and ionic ***,even with the low content of UIOSNa fillers,a high ionic conductivity of 6.62×10^(-4) S·cm^(-1) at 60℃ and a transference number of 0.67 for the special designed composite electrolyte are *** assembled all-solid-state sodium cell exhibits a remarkable rate performance for 500 cycles with 95.96%capacity retention at a high current rate of 4 *** corresponding pouch cell can stably work for 1000 cycles with 97.03%capacity retention at 1 C,which is superior to most of the reported composite electrolytes in the literature.

关键词： solid state sodium battery composite electrolyte rate performance cycle life

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Dual-compressed photoacoustic single-pixel imaging

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National science Review 2023年第1期10卷 187-195页

作者： Yuning Guo Baowen Li Xiaobo Yin Department of Mechanical Engineering University of Colorado Department of Material Science and Engineering Department of Physics Shenzhen Institute for Quantum Science and Engineering Southern University of Science and Technology Materials Science and Engineering Program University of Colorado

Photoacoustic imaging,an acoustic imaging modality with potentially optical resolution in an optical turbid medium,has attracted great ***,the convergence of wavefront optimization and raster scanning in computational photoacoustic imaging leads to the challenge of fast mapping,especially for a spatial resolution approaching the acoustic deep-subwavelength *** a sparse sampling paradigm,compressive sensing has been applied in numerous fields to accelerate data acquisition without significant quality *** this work,we propose a dual-compressed approach for photoacoustic surface tomography that enables high-efficiency imaging with 3D spatial resolution unlimited by the acoustics in a turbid *** dual-compressed photoacoustic imaging with single-pixel detection,enabled by spatially optical modulation with synchronized temporally photoacoustic coding,allows decoding of the fine optical information from the modulated acoustic signal even when the variance of original photoacoustic signals is *** perform a proof-of-principle numerical demonstration of dual-compressed photoacoustic imaging, that resolves acoustic sub-acoustic-wavelength details with a significantly reduced number of measurements,revealing the potential for dynamic *** dual-compressed concept,which transforms unobtrusive spatial difference into spatio-temporal detectable information,can be generalized to other imaging modalities to re alize efficient,high-spatial-resolution imaging.

关键词： photoacoustic imaging compressive sensing single-pixel imaging surface tomography

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Preparation and performance of novel magnetic phase-change-microcapsule-supported Bi_(2)WO_(6)catalyst

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Chinese Chemical Letters 2024年第3期35卷 158-161页

作者： Zhuoni Jiang Zhiqing Ge Shuo Yan Jingjing Shu Mozhen Wang Xuewu Ge Key Laboratory of Precision and Intelligent Chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China School of Materials Science and Engineering Southwest University of Science and TechnologyMianyang 621010China

The design and synthesis of novel photocatalyst with self-temperature control function is an important topic in the field of advanced environmental functional *** this work,submicron-sized magnetic phase change microcapsules composed of paraffin core and Fe_(3)O_(4)-loaded silica shell are prepared,on which the Bi_(2)WO_(6)crystals is grown in situ through hydrothermal reaction to obtain novel magnetic phase-change-microcapsule-supported Bi_(2)WO_(6)catalyst(MP@FS/BWO).The MP@FS/BWO has a paraffin encapsulation ratio of 57.1%,and the phase change enthalpy of 105.1 J/g in a temperature range of 50–60℃,which endows the MP@FS/BWO with a certain self-temperature regulation ***@FS/BWO shows excellent catalytic performance in the decomposition of rhodamine B under the simulated sunlight *** the light source is turned off,it still has good catalytic ability by maintaining high temperature due to its temperature control function based on the phase transition *** MP@FS/BWO can be easily recycled by magnetic separation and shows good structural stability and *** work provides a new idea for the development of long-effect and energy-saving outdoor photocatalysts.

关键词： Photocatalyst Phase change microcapsules Self-temperature regulation Bismuth tungstate Magnetic separation

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In-situ understanding on the formation of fibrillar morphology in green solvent processed all-polymer solar cells

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National science Review 2024年第12期11卷 244-253页

作者： Ruijie Ma Hongxiang Li Top Archie Dela Pe?a Heng Wang Cenqi Yan Pei Cheng Jiaying Wu Gang Li Department of Electrical and Electronic Engineering Research Institute for Smart Energy (RISE)Photonic Research Institute (PRI) The Hong Kong Polytechnic University College of Polymer Science and Engineering State Key Laboratory of Polymer Materials Engineering Sichuan University Function Hub Advanced Materials Thrust The Hong Kong University of Science and Technology

Solid additive engineering has been intensively explored on morphology tuning for highly efficient all-polymer solar cells（all-PSCs）, a promising photovoltaic technology towards multi-scenario *** the nano-fibrillar network of the active layer induced by additive treatment is confirmed as the key factor for power conversion efficiency（PCE） of all-PSCs, its formation mechanism is not clearly revealed,for lack of precise and convincing real-time observation of crystallization and phase separation during the liquid-to-solid transition process of spin-coating. Herein we report an in-situ grazing incidence wide-angle/small-angle X-ray scattering（GIWAXS/GISAXS） screening that reveals the fact that naphthalene derived solid additives can suppress the aggregation of the polymer acceptor（PY-IT） at the beginning stage of spin coating, which provides sufficient time and space for the polymer donor（PM6） to form the fibril structure. Moreover, guided by this knowledge, a ternary all-polymer system is proposed,which achieves cutting-edge level PCEs for both small-area（0.04 cm2）(also decent operational stability)and large-area（1 cm2） devices.

关键词： all-polymer solar cells morphology screening naphthalene-based solid additives phase segregation

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Improving Thermal-oxidative Aging Resistance of Styrene-butadiene Rubber by Antioxidant Loaded Silica Aerogel

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Chinese Journal of polymer science 2024年第8期42卷 1198-1209页

作者： Xue-Fei Ping Yu Wang Lu Liu Fu-Yong Liu Hong-Wei He Pi Wang Wen-Wen Yu Qiang Zheng College of Materials Science and Engineering Taiyuan University of TechnologyTaiyuan 030024China Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering Taiyuan 030032China Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310058China

The antioxidant N-isopropyl-N'-phenyl-p-phenylenediamine(4010NA)was dissolved in ethanol and impregnated into silica aerogel(SAG)via vacuum-pressure cycles,yielding composite particles(A-N)with enhanced sustained-release and reinforcing *** effect of A-N on the mechanical properties and thermal-oxidative aging resistance of styrene-butadiene rubber(SBR)vulcanizates was *** and BET assessments indicated that the loading efficiency of 4010NA in SAG reached 14.26%within ethanol's solu bility *** A-N into SBR vulcanizates significantly elevated tensile strength by 17.5%and elongation at break by 41.9%over those with fumed silica and ***,A-N notably enhanced the thermal-oxidative aging resistance of *** aging for 96 h at 100℃,the tensile strength and elongation at break of SBR with A-N sustained 70.09%and 58.61%of their initial values,respectively,with the retention rate of elongation at break being 62.8%higher than that of SBR with fumed silica and free *** study revealed that A-N composite particles significantly inhibited the crosslinking in SBR's molecular chains,reducing hardening and embrittlement during later thermal-oxidative aging stages.

关键词： Styrene-butadiene rubber Silica aerogel Loading modification Thermal-oxidative aging

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Liquid Metal Grid Patterned Thin Film Devices Toward Absorption‑Dominant and Strain‑Tunable Electromagnetic Interference Shielding

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Nano-Micro Letters 2024年第11期16卷 541-553页

作者： Yuwen Wei Priyanuj Bhuyan Suk Jin Kwon Sihyun Kim Yejin Bae Mukesh Singh Duy Thanh Tran Minjeong Ha Kwang‑Un Jeong Xing Ma Byeongjin Park Sungjune Park Department of Polymer‑Nano Science and Technology Department of Nano Convergence EngineeringJeonbuk National UniversityJeonju 54896Republic of Korea School of Chemical Engineering Sungkyunkwan University(SKKU)Suwon 16419Republic of Korea Composites Research Division Korea Institute of Materials ScienceChangwon 51508Republic of Korea School of Materials Science and Engineering Gwangju Institute of Science and TechnologyGwangju 61005Republic of Korea School of Materials Science and Engineering and Sauvage Laboratory for Smart MaterialsHarbin Institute of Technology(Shenzhen)ShenzhenGuangdong 518055People’s Republic of China

The demand of high-performance thin-film-shaped deformable electromagnetic interference(EMI)shielding devices is increasing for the next generation of wearable and miniaturized soft *** highly reflective conductive materials can effectively shield EMI,they prevent deformation of the devices owing to rigidity and generate secondary electromagnetic pollution ***,soft and stretchable EMI shielding thin film devices with absorption-dominant EMI shielding behavior is *** devices consist of liquid metal(LM)layer and LM grid-patterned layer separated by a thin elastomeric film,fabricated by leveraging superior adhesion of aerosol-deposited LM on *** devices demonstrate high electromagnetic shielding effectiveness(SE)(SE_(T) of up to 75 dB)with low reflectance(SER of 1.5 dB at the resonant frequency)owing to EMI absorption induced by multiple internal reflection generated in the LM grid ***,the excellent stretchability of the LM-based devices facilitates tunable EMI shielding abilities through grid space adjustment upon strain(resonant frequency shift from 81.3 to 71.3 GHz@33%strain)and is also capable of retaining shielding effectiveness even after multiple strain *** newly explored device presents an advanced paradigm for powerful EMI shielding performance for next-generation smart electronics.

关键词： Absorption-dominant electromagnetic interference shielding Liquid metals Soft and stretchable electronics Thin film devices Tunable electromagnetic interference shielding

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Facile Synthesis of Polycarbonate Diol via Copolymerization of CO_(2) and Cyclohexene Oxide Catalysed by a Combination of One-Component Phosphonium Borane Lewis Pair and Water

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Chinese Journal of polymer science 2023年第5期41卷 735-744,I0009页

作者： Xiao-Wu Wang Ji-Wen Hui Yu-Tao Li Yan-Ru Gu Zhi-Bo Li State Key Laboratory Base of Eco-Chemical Engineering/College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042China Key Laboratory of Biobased Polymer Materials Shandong Provincial Education Department/School of Polymer Science and EngineeringQingdao University of Science and TechnologyQingdao 266042China

Well-defined polycarbonate diol was successfully synthesized through a strategy using a combination of organocatalyst and *** strategy was less developed in organocatalyzed polymerization and frequently regarded as side ***,one-component phosphonium borane Lewis pairs PB1-PB8 were successfully applied in the copolymerization of CO_(2) and cyclohexene oxide(CHO)to generate poly(CHO-alt-CO_(2))carbonate(PCHC).Parameters of linker length and counter anion effects on the catalyst activity were *** was found that Lewis pair PB3 served as a dual initiator and catalyst in the copolymerization of CHO and CO_(2) with or without the presence of *** contrast,Lewis pair PB8 can serve as a true catalyst for the preparation of well-definedα,ω-hydroxyl PCHC *** was achieved by introducing a labile CF3COO group as counter anion through anion exchange reaction while water molecules acted as chain transfer *** function of trifluoroacetate group in the polymerization process was investigated in detail and possible mechanism was *** changing the amount of water and catalyst loading,PCHC diols with varied molecular weight(1.5 kg/mol to 7.5 kg/mol),low dispersities(D<1.2)and carbonate content(>99%)could be easily *** low molecular weight PCHC diol was used as a bifunctional macroinitiator for the ring-opening polymerization of L-lactide(LLA)to afford ABA triblock copolymer in one-pot synthesis.

关键词： Polycarbonate Phosphonium borane Lewis pair CO_(2)utilization Organocatalysis Ring-opening polymerization

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Highly active organocatalyst from a trivalent phosphazenium salt for ring-opening copolymerization of epoxides and cyclic anhydrides enhanced by hydrogen bonding interactions

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science China Chemistry 2024年第9期67卷 3111-3120页

作者： Chunhuan Jiang Junqi Wang Xiaoyu Liu Xiaoxia You Ronglin Zhong Chuanli Ren Zhibo Li Key Laboratory of Biobased Polymer Materials Shandong Provincial Education DepartmentCollege of Polymer Science and EngineeringQingdao University of Science and TechnologyQingdao 266042China College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042China Laboratory of Theoretical and Computational Chemistry Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130012China

It is highly desirable to develop simple organocatalysts for the controlled ring-opening alternating copolymerization(ROAC)of epoxides and cyclic anhydrides,leading to high molecular weight ***,a phosphazenium salt,namely tri[tris(dimethylamino)phosphoranylidenamino]phosphonium chloride(P_(4)^(+)Cl^(-)),is developed as a catalyst for the ROAC of epoxides and cyclic ***,the combination of P_(4)^(+)Cl^(-)with a protonic initiator,such as 1,4-benzenedimethanol(BDM)exhibited high efficiency in the copolymerization of propylene oxide(PO)and phthalic anhydride(PA).This led to the production of polyester with an exceptional high molecular weight(M_n)of up to 126 k Da,which represented a rare example of poly(PO-alt-PA)with Mnsurpassing 100 k *** that the core P atom is trivalent status and the tris[tris(dimethylamino)]phosphoranyl group will share one proton in the P_(4)^(+)Cl^(-)*** combined with protonic species,the P_(4)^(+)Cl^(-)will not only serve as a proton acceptor but also as a hydrogen bonding donor for the cyclic ***,it was assumed that the P_(4)^(+)plus proton served dual role in mimic of base/urea pair to effectively catalyze ROAC,which was supported by density functional theory(DFT)calculations.

关键词： ring-opening copolymerization organocatalyst epoxides cyclic anhydrides phosphazenium salt

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Sequence structure controllable polymerization-induced self-assembly

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science China Chemistry 2024年第1期67卷 390-397页

作者： Zi-Xuan Chang Ren-Man Zhu Chun-Yan Hong Wen-Jian Zhang Department of Polymer Science and Engineering University of Science and Technology of ChinaHefei 230026China Institute of Physical Science and Information Technology Anhui UniversityHefei 230601China Key Laboratory of Environment-Friendly Polymeric Materials of Anhui Province Anhui UniversityHefei 230601China

polymerization-induced self-assembly(PISA)combines synthesis and self-assembly of artificial polymers in one-pot,which brings us one step closer to emulating ***,the reported PISA formulations primarily focus on developing nano-objects with new chemical compositions and rarely on structural regulation of polymers with specific ***,sequence structure controllable polymerization-induced self-assembly(SCPISA)is reported by using 7-(2-methacryloyloxyethoxy)-4-methylcoumarin(CMA)as a *** the copolymerization of 2-hydroxyethyl methacrylate(HEMA)and CMA,controlled incorporation of CMA units into the polymer chains can be realized by programmable light/heat ***-based P(HEMA-co-CMA)copolymers with the same composition but different sequence structures generate a range of ***,the morphologies of the resultant nano-objects can also be controlled by regulating the feed molar ratio of CMA and HEMA,which is similar to the conventional PISA,but the synthesis procedure is obviously simplified in *** versatility of the methodology is further demonstrated by the fabrication of different functional nano-objects with sequence structure-dependent morphologies in SCPISA systems with different functional monomers.

关键词： polymerization-induced self-assembly sequence-controlled polymers PET-RAFT polymerization

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