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Highly Aligned Graphene Aerogels for Multifunctional Composites

Nano-Micro Letters 2024年第6期16卷 276-342页

作者： Ying Wu Chao An Yaru Guo Yangyang Zong Naisheng Jiang Qingbin zheng zhong‑zhen yu Beijing Advanced Innovation Center for Materials Genome Engineering School of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing 100083People’s Republic of China Institute of Materials Intelligent Technology Liaoning Academy of MaterialsShenyang 110004People’s Republic of China School of Science and Engineering The Chinese University of Hong KongShenzhenShenzhenGuangdong 518172People’s Republic of China State Key Laboratory of Organic‑Inorganic Composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China

Stemming from the unique in-plane honeycomb lattice structure and the sp^(2)hybridized carbon atoms bonded by exceptionally strong carbon–carbon bonds,graphene exhibits remarkable anisotropic electrical,mechanical,and thermal properties.To maximize the utilization of graphene’s in-plane properties,pre-constructed and aligned structures,such as oriented aerogels,films,and fibers,have been designed.The unique combination of aligned structure,high surface area,excellent electrical conductivity,mechanical stability,thermal conductivity,and porous nature of highly aligned graphene aerogels allows for tailored and enhanced performance in specific directions,enabling advancements in diverse fields.This review provides a comprehensive overview of recent advances in highly aligned graphene aerogels and their composites.It highlights the fabrication methods of aligned graphene aerogels and the optimization of alignment which can be estimated both qualitatively and quantitatively.The oriented scaffolds endow graphene aerogels and their composites with anisotropic properties,showing enhanced electrical,mechanical,and thermal properties along the alignment at the sacrifice of the perpendicular direction.This review showcases remarkable properties and applications of aligned graphene aerogels and their composites,such as their suitability for electronics,environmental applications,thermal management,and energy storage.Challenges and potential opportunities are proposed to offer new insights into prospects of this material.

关键词： Highly aligned graphene aerogels Quantitative characterization of alignment Multifunctional composites Anisotropic properties Multifunctional applications

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Direct ink writing of multifunctional gratings with gel-like MXene/norepinephrine ink for dynamic electromagnetic interference shielding and patterned Joule heating

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Nano Research 2024年第3期17卷 1585-1594页

作者： Pei-Zhu Jiang Zhiming Deng Peng Min Lvxuan Ye Cheng-Zhang Qi Hao-yu Zhao Ji Liu Hao-Bin Zhang zhong-zhen yu Beijing Key Laboratory of Advanced Functional Polymer Composites Beijing University of Chemical TechnologyBeijing 100029China State Key Laboratory of Organic-Inorganic Composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China School of Chemistry CRANN and AMBERTrinity College DublinDublin D02PN40Ireland

Intelligent electromagnetic interference(EMI)shielding modulators with a wide tuning range and cyclic stability are urgently needed but their fabrication remains challenging.A gel-like MXene/norepinephrine ink is developed and multifunctional MXene gratings with wide EMI shielding effectiveness(SE)tuning range,superior reversibility,and high mechanical flexibility are constructed by direct ink writing approach for dynamic EMI shielding and patterned Joule heating applications.The modulable MXene/norepinephrine grating with a high conductivity of 3510 S·cm-1 can conveniently realize the seamless modulation of the EMI SE by adjusting the angle between the MXene grating filaments and the electric field of the incident electromagnetic waves,offering highly reversible switching between shielding“On”(28.0 dB)and“Off”(0.5 dB)states.Notably,due to the optimized integration of the MXene ink and the rationally designed pattern,a superior specific EMI SE of 95,688.2 dB·cm^(2)·g^(-1) is achieved in the“On”state.Furthermore,the MXene/norepinephrine ink can be used to fabricate many complex patterned gratings with superior stability,instant responsibility,and superb mechanical flexibility,exhibiting a unique patterned Joule heating behavior.Direct writing of multifunctional gratings paves a means for developing intelligent EMI shielding materials,wearable electronic devices,and advanced thermal management materials.

关键词： MXene ink direct ink writing electromagnetic interference shielding multifunctional gratings Joule heating

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Efficient Preconstruction of Three‑Dimensional Graphene Networks for Thermally Conductive Polymer Composites

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Nano-Micro Letters 2022年第8期14卷 72-111页

作者： Hao‑yu Zhao Ming‑yuan yu Ji Liu Xiaofeng Li Peng Min zhong‑zhen yu Beijing Key Laboratory of Advanced Functional Polymer Composites Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China College of Materials Science and Engineering Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China School of Chemistry CRANN and AMBERTrinity College DublinDublinIreland

Electronic devices generate heat during operation and require efficient thermal management to extend the lifetime and prevent performance degradation.Featured by its exceptional thermal conductivity,graphene is an ideal functional filler for fabricating thermally conductive polymer composites to provide efficient thermal management.Extensive studies have been focusing on constructing graphene networks in polymer composites to achieve high thermal conductivities.Compared with conventional composite fabrications by directly mixing graphene with polymers,preconstruction of three-dimensional graphene networks followed by backfilling polymers represents a promising way to produce composites with higher performances,enabling high manufacturing flexibility and controllability.In this review,we first summarize the factors that affect thermal conductivity of graphene composites and strategies for fabricating highly thermally conductive graphene/polymer composites.Subsequently,we give the reasoning behind using preconstructed three-dimensional graphene networks for fabricating thermally conductive polymer composites and highlight their potential applications.Finally,our insight into the existing bottlenecks and opportunities is provided for developing preconstructed porous architectures of graphene and their thermally conductive composites.

关键词： Graphene networks Thermal conductivity Thermal interface materials Phase change composites Anisotropic aerogels

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Super-Tough and Environmentally Stable Aramid Nanofiber@MXene Coaxial Fibers with Outstanding Electromagnetic Interference Shielding Efficiency

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Nano-Micro Letters 2022年第7期14卷 72-85页

作者： Liu-Xin Liu Wei Chen Hao-Bin Zhang Lvxuan Ye zhenguo Wang yu Zhang Peng Min zhong-zhen yu State Key Laboratory of Organic-Inorganic Composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China Beijing Key Laboratory of Advanced Functional Polymer Composites Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China

Although electrically conductive and hydrophilic MXene sheets are promising for multifunctional fibers and electronic textiles,it is still a challenge to simultaneously enhance both conductivity and mechanical properties of MXene fibers because of the high rigidity of MXene sheets and insufficient inter-sheet interactions.Herein,we demonstrate a core-shell wet-spinning methodology for fabricating highly conductive,super-tough,ultra-strong,and environmentally stable Ti_(3)C_(2)T_(x) MXene-based core-shell fibers with conductive MXene cores and tough aramid nanofiber(ANF)shells.The highly orientated and low-defect structure endows the ANF@MXene core-shell fiber with supertoughness of~48.1 MJ m^(-3),high strength of~502.9 MPa,and high conductivity of~3.0×10^(5)S m^(-1).The super-tough and conductive ANF@MXene fibers can be woven into textiles,exhibiting an excellent electromagnetic interference(EMI)shielding efficiency of 83.4 dB at a small thickness of 213μm.Importantly,the protection of the ANF shells provides the fibers with satisfactory cyclic stability under dynamic stretching and bending,and excellent resistance to acid,alkali,seawater,cryogenic and high temperatures,and fire.The oxidation resistance of the fibers is demonstrated by their wellmaintained EMI shielding performances.The multifunctional core-shell fibers would be highly promising in the fields of EMI shielding textiles,wearable electronics and aerospace.

关键词： Core-shell fibers MXene sheets Electromagnetic interference shielding Aramid nanofibers Super-toughness

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Constructing central hollow cylindrical reduced graphene oxide foams with vertically and radially orientated porous channels for highly efficient solar-driven water evaporation and purification

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Nano Research 2023年第5期16卷 6343-6352页

作者： Changjun Li Wei Li Hao-yu Zhao Xin-yue Feng Xiaofeng Li zhong-zhen yu State Key Laboratory of Organic-Inorganic Composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China Beijing Key Laboratory of Advanced Functional Polymer Composites Beijing University of Chemical TechnologyBeijing 100029China College of Materials Science and Engineering Shandong University of Science and TechnologyQingdao 266590China

Although solar steam generation is an eco-friendly approach for desalinating seawater and purifying wastewater,there are still issues on how to improve the efficiency of solar energy utilization and accelerate the water and heat transport inside the solardriven water evaporators.Herein,we design a central hollow cylindrical reduced graphene oxide(RGO)foam with vertically and radially orientated channels as a solar steam generation device for efficient water evaporation and purification.The vertically aligned porous channels accelerate upward transport of water to the top evaporation surface,while the radially aligned porous channels facilitate water transport and heat transfer along the radial directions for fully utilizing the heat accumulated inside the central cylindrical hole of the foam.The central hole of the foam plays a highly positive role in accumulating more heat for accelerating the water evaporation,the newly generated inner sidewall resulted from the central hole can gain extra thermal energy from surrounding environment in the same way as the outer sidewall of the foam due to the surface cooling effect of the water evaporation.As a result,the vertically and radially aligned RGO foam evaporator with central hollow cylinder achieves a high solar steam generation rate of 2.32 kg·m^(−2)·h^(−1)with an exceptional energy conversion efficiency of 120.9%under 1-sun irradiation,superior to the vertically aligned RGO foam without the central hole(1.83 kg·m^(−2)·h^(−1),96.9%)because of the enhanced water and heat transfer inside the porous channels,the efficient utilization of environmental energy.

关键词： hollow cylindrical foams reduced graphene oxide solar steam generation water evaporation rate seawater desalination

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Strong and conductive reduced graphene oxide-MXene porous films for efficient electromagnetic interference shielding

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Nano Research 2022年第6期15卷 4916-4924页

作者： yu Zhang Ming-Ke Xu zhenguo Wang Tianyu Zhao Liu-Xin Liu Hao-Bin Zhang zhong-zhen yu State Key Laboratory of Organic-Inorganic Composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China Beijing Key Laboratory of Advanced Functional Polymer Composites Beijing University of Chemical TechnologyBeijing 100029China

Lightweight,flexible,and electrically conductive porous films are promising for efficient electromagnetic interference(EMI)shielding.However,the mechanical and electrical properties of porous films are far from optimum.Herein,we fabricate mechanically flexible and electrically conductive reduced graphene oxide(rGO)-Ti_(3)C_(2)T_(x)MXene(rG-M)porous films with optimized continuous cellular morphology by a controlled hydrazine foaming process.The presence of MXene prevents excessive expansion of the rG-M film,improves the electron conduction paths,and enhances the mechanical properties.The resultant rG-M porous film has superior mechanical and electric performances compared to its rGO counterpart,giving one of the highest tensile strengths(24.5 MPa)among the porous films,a high electrical conductivity of 74.4 S·cm^(−1),and an excellent broadband EMI shielding from 8 to 26.5 GHz.A high EMI shielding effectiveness of 52.6 dB is achieved for the porous film by adjusting its thickness and treatment procedure,providing a feasible fabrication route for lightweight and high-performance EMI shielding materials.

关键词： graphene MXene electromagnetic interference shielding porous films electrical conductivity

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Multifunctional Waterborne Polyurethane Nanocomposite Films with Remarkable Electromagnetic Interference Shielding,Electrothermal and Solarthermal Performances

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Chinese Journal of Polymer Science 2023年第2期41卷 267-277页

作者： Ming-Ke Xu Xin-Jie Luo Hao-Bin Zhang yu Zhang Lulu Li Xin-Feng Zhou zhong-zhen yu Beijing Key Laboratory of Advanced Functional Polymer Composites Beijing University of Chemical TechnologyBeijing100029China State Key Laboratory of Organic-Inorganic Composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing100029China

To impart polymers with high electrical conductivity and satisfactory electromagnetic interference shielding efficiency,it is crucial to efficiently construct interconnecting networks of conductive nanofillers in polymer matrices.Herein,on the basis of the three-dimensional(3D)skeleton and volume-exclusion effect of silane-modified tetra-needle ZnO(ST-ZnO)whiskers and the high conductivity of two-dimensional MXene nanosheets,multifunctional MXene/ST-ZnO/waterborne polyurethane(MTW)nanocomposite films are fabricated by coating of MXene on ST-ZnO followed by compounding with waterborne polyurethane.The 3D four-needles of the whiskers facilitate the formation of an interconnecting network in the waterborne polyurethane matrix,while the coating of MXene efficiently makes the interconnecting network of the whiskers conductive at a low amount of the MXene.The resultant MTW ternary nanocomposite film exhibits not only a high electrical conductivity of 4.8×10^(4)S/m,but also an excellent electromagnetic interference shielding effectiveness of over 70 dB in the X-band at a low thickness of 100µm.In addition,the ternary film also exhibits outstanding Joule heating performances with an equilibrium temperature of 113℃at a low driving voltage of 3 V.The multifunctional nanocomposite films are promising for applications in portable and wearable electronics and flexible electromagnetic interference shielding devices.

关键词： Electrical conductivity Electromagnetic interference shielding Nanocomposite films Waterborne polyurethane MXene nanosheets

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Highly conductive calcium ion-reinforced MXene/sodium alginate aerogel meshes by direct ink writing for electromagnetic interference shielding and Joule heating

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Journal of Materials Science & Technology 2023年第4期135卷 213-220页

作者： Cheng-Zhang Qi Xinyu Wu Ji Liu Xin-Jie Luo Hao-Bin Zhang zhong-zhen yu Beijing Key Laboratory of Advanced Functional Polymer Composites Beijing University of Chemical TechnologyBeijing 100029China State Key Laboratory of Organic-Inorganic Composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China School of Chemistry CRANN and AMBERTrinity College DublinD2DublinIreland

Although MXene sheets possess high electrical conductivity and rich surface chemistry and are well suit-able for fabricating electrically conductive nanocomposites for electromagnetic interference(EMI)shield-ing applications,it remains challenging for MXene nanocomposites to achieve tunable EMI shielding per-formances and customized geometries.Herein,an aqueous MXene/sodium alginate ink is developed to print aerogel meshes with customized geometries using a direct ink writing approach.An ion-enhanced strategy is proposed to reinforce the printed aerogel meshes by multi-level cross-linking.The resultant 3D printed aerogel mesh exhibits an ultrahigh electrical conductivity of 2.85×10^(3)S m^(−1),outstanding mechanical properties,and excellent structural stability in wet environment.More importantly,a wide range of tunable EMI shielding efficiencies from 45 to 100 dB is achieved by the structural design of the 3D printed ion-enhanced MXene/sodium alginate aerogel meshes.As a Joule heater,in addition,the printed aerogel meshes can achieve a wide temperature range of 40-135℃at low driving voltages.This work demonstrates a direct ink writing approach for the fabrication of ion-enhanced MXene/sodium al-ginate aerogel meshes with tunable EMI shielding properties and multi-functionalities for applications in many scenarios.

关键词： MXene inks Aerogels Electromagnetic interference shielding Direct ink writing Joule heating

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Electrically conductive and highly compressible anisotropic MXene-wood sponges for multifunctional and integrated wearable devices

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Journal of Materials Science & Technology 2023年第13期144卷 102-110页

作者： Dekui Song Mei-Jiao Zeng Peng Min Xue-Qin Jia Fu-Lin Gao zhong-zhen yu Xiaofeng Li State Key Laboratory of Organic-Inorganic Composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China Beijing Key Laboratory of Advanced Functional Polymer Composites Beijing University of Chemical TechnologyBeijing 100029China College of Chemistry Beijing Normal UniversityBeijing100875China

Although piezoresistive sensors have wide applications in human motion detection and wearable elec-tronics,it is still a challenge to produce multifunctional and integrated sensors with wide working ranges and linear sensing responses.Herein,electrically conductive,highly compressible,and structurally anisotropic MXene-wood(MW)sponges are fabricated by converting balsa wood blocks to compressible wood sponges with extremely low density and highly anisotropic porous structure,followed by deco-rating with conductive MXene sheets.The MW sponge is utilized to assemble a piezoresistive sensor with a large working range of 0-25 kPa,wide linear sensing ranges of 5%-50%and 0-180°,and excellent long-term reliability under a bending angle of 30°for 5000 cycles.Additionally,the sensor is suitable for monitoring practical human physiological signals including pulse beating,and finger and wrist bending.An all-MW sponge-based multifunctional and integrated sensing system is constructed by integrating the MW sponge piezoresistive sensor,the MW sponge-based solid-state supercapacitor,and the MW sponge electrophysiological electrodes.The sensing system can concurrently detect surface electromyogram and tactile pressures,and hence realize real-time closed-loop controls.The multifunctional and integrated MW sponge sensing system would have great potentials in real-time pressure recognition and human-machine interfaces.

关键词： MXene sheets Wood sponges Piezoresistive sensors Compressibility

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3D Lamellar-Structured Graphene Aerogels for Thermal Interface Composites with High Through-Plane Thermal Conductivity and Fracture Toughness

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Nano-Micro Letters 2021年第2期13卷 13-27页

作者： Pengfei Liu Xiaofeng Li Peng Min Xiyuan Chang Chao Shu yun Ding zhong-zhen yu Beijing Key Laboratory of Advanced Functional Polymer Composites Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China State Key Laboratory of Organic-Inorganic Composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China

Although thermally conductive graphene sheets are efficient in enhancing in-plane thermal conductivities of polymers,the resulting nanocomposites usually exhibit low through-plane thermal conductivities,limiting their application as thermal interface materials.Herein,lamellarstructured polyamic acid salt/graphene oxide(PAAS/GO)hybrid aerogels are constructed by bidirectional freezing of PAAS/GO suspension followed by lyophilization.Subsequently,PAAS monomers are polymerized to polyimide(PI),while GO is converted to thermally reduced graphene oxide(RGO)during thermal annealing at 300℃.Final graphitization at 2800℃ converts PI to graphitized carbon with the inductive effect of RGO,and simultaneously,RGO is thermally reduced and healed to high-quality graphene.Consequently,lamellar-structured graphene aerogels with superior through-plane thermal conduction capacity are fabricated for the first time,and its superior through-plane thermal conduction capacity results from its vertically aligned and closely stacked high-quality graphene lamellae.After vacuum-assisted impregnation with epoxy,the resultant epoxy composite with 2.30 vol% of graphene exhibits an outstanding through-plane thermal conductivity of as high as 20.0 W m^−1 K^−1,100 times of that of epoxy,with a record-high specific thermal conductivity enhancement of 4310%.Furthermore,the lamellar-structured graphene aerogel endows epoxy with a high fracture toughness,~1.71 times of that of epoxy.

关键词： Anisotropic aerogels Graphene Thermal conductivity Epoxy composites Fracture toughness

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