Laser‐Induced Freestanding Graphene Papers: A New Route of Scalable Fabrication with Tunable Morphologies and Properties for Multifunctional Devices and Structures

The recently emergent laser‐induced graphene (LIG) technology has endowed the fabrication of smart devices with one‐step processing and scalable/designable features. Graphene paper (GP), an important architecture of 2D layered carbon, however, is never produced through LIG. Herein, a novel strategy is reported for production of freestanding GP through LIG technology. It is first determined that the unique spatial configuration of polyimide (PI) paper is critical for the preparation of GP without the appearance of intense shape distortion. Benefiting from the mechanism, the as‐produced laser‐induced graphene paper (LIGP) is foldable, trimmable, and integratable to customized shapes and structures with the largest dimension of 40 × 35 cm². Based on the processing–structure–property relationship study, one is capable of controlling and tuning various physical and chemical properties of LIGPs, rendering them unique for assembling flexible electronics and smart structures, e.g., human/robotic motion detectors, liquid sensors, water–oil separators, antibacterial media, and flame retardant/deicing/self‐sensing composites. With the key findings, the escalation of LIGP for commercialization, roll‐to‐roll manufacturing, and multidisciplinary applications are highly expected.     

Laser‐Induced Graphene: From Discovery to Translation

Laser‐induced graphene (LIG) is a 3D porous material prepared by direct laser writing with a CO₂ laser on carbon materials in ambient atmosphere. This technique combines 3D graphene preparation and patterning into a single step without the need for wet chemical steps. Since its discovery in 2014, LIG has attracted broad research interest, with several papers being published per month using this approach. These serve to delineate the mechanism of the LIG‐forming process and to showcase the translation into many application areas. Herein, the strategies that have been developed to synthesize LIG are summarized, including the control of LIG properties such as porosity, composition, and surface characteristics, and the advancement in methodology to convert diverse carbon precursors into LIG. Taking advantage of the LIG properties, the applications of LIG in broad fields, such as microfluidics, sensors, and electrocatalysts, are highlighted. Finally, future development in biodegradable and biocompatible materials is briefly discussed.     

Laser‐Induced Graphene Formation on Wood

Wood as a renewable naturally occurring resource has been the focus of much research and commercial interests in applications ranging from building construction to chemicals production. Here, a facile approach is reported to transform wood into hierarchical porous graphene using CO₂ laser scribing. Studies reveal that the crosslinked lignocellulose structure inherent in wood with higher lignin content is more favorable for the generation of high‐quality graphene than wood with lower lignin content. Because of its high electrical conductivity (≈10 Ω per square), graphene patterned on wood surfaces can be readily fabricated into various high‐performance devices, such as hydrogen evolution and oxygen evolution electrodes for overall water splitting with high reaction rates at low overpotentials, and supercapacitors for energy storage with high capacitance. The versatility of this technique in formation of multifunctional wood hybrids can inspire both research and industrial interest in the development of wood‐derived graphene materials and their nanodevices.     

Oxidized Laser‐Induced Graphene for Efficient Oxygen Electrocatalysis

An efficient metal‐free catalyst is presented for oxygen evolution and reduction based on oxidized laser‐induced graphene (LIG‐O). The oxidation of LIG by O₂ plasma to form LIG‐O boosts its performance in the oxygen evolution reaction (OER), exhibiting a low onset potential of 260 mV with a low Tafel slope of 49 mV dec^?1, as well as an increased activity for the oxygen reduction reaction. Additionally, LIG‐O shows unexpectedly high activity in catalyzing Li₂O₂ decomposition in Li‐O₂ batteries. The overpotential upon charging is decreased from 1.01 V in LIG to 0.63 V in LIG‐O. The oxygen‐containing groups make essential contributions, not only by providing the active sites, but also by facilitating the adsorption of OER intermediates and lowering the activation energy.     

Flexible,Stretchable, and Transparent Planar Microsupercapacitors Based on 3D Porous Laser‐Induced Graphene

The graphene with 3D porous network structure is directly laser‐induced on polyimide sheets at room temperature in ambient environment by an inexpensive and one‐step method, then transferred to silicon rubber substrate to obtain highly stretchable, transparent, and flexible electrode of the all‐solid‐state planar microsupercapacitors. The electrochemical capacitance properties of the graphene electrodes are further enhanced by nitrogen doping and with conductive poly(3,4‐ethylenedioxythiophene) coating. With excellent flexibility, stretchability, and capacitance properties, the planar microsupercapacitors present a great potential in fashionable and comfortable designs for wearable electronics.     

Laser‐Induced Direct Graphene Patterning and Simultaneous Transferring Method for Graphene Sensor Platform

General methods utilized in the fabrication of graphene devices involve graphene transferring and subsequent patterning of graphene via multiple wet‐chemical processes. In the present study, a laser‐induced pattern transfer (LIPT) method is proposed for the transferring and patterning of graphene in a single processing step. Via the direct graphene patterning and simultaneous transferring, the LIPT method greatly reduces the complexity of graphene fabrication while augmenting flexibility in graphene device design. Femtosecond laser ablation under ambient conditions is employed to transfer graphene/PMMA microscale patterns to arbitrary substrates, including a flexible film. Suspended cantilever structures are also demonstrated over a prefabricated trench structure via the single‐step method. The feasibility of this method for the fabrication of functional graphene devices is confirmed by measuring the electrical response of a graphene/PMMA device under laser illumination.     

Laser‐Induced Graphene in Controlled Atmospheres: From Superhydrophilic to Superhydrophobic Surfaces

The modification of graphene‐based materials is an important topic in the field of materials research. This study aims to expand the range of properties for laser‐induced graphene (LIG), specifically to tune the hydrophobicity and hydrophilicity of the LIG surfaces. While LIG is normally prepared in the air, here, using selected gas atmospheres, a large change in the water contact angle on the as‐prepared LIG surfaces has been observed, from 0° (superhydrophilic) when using O₂ or air, to >150° (superhydrophobic) when using Ar or H₂. Characterization of the newly derived surfaces shows that the different wetting properties are due to the surface morphology and chemical composition of the LIG. Applications of the superhydrophobic LIG are shown in oil/water separation as well as anti‐icing surfaces, while the versatility of the controlled atmosphere chamber fabrication method is demonstrated through the improved microsupercapacitor performance generated from LIG films prepared in an O₂ atmosphere.     

Thermal Shock Synthesis of Nanocatalyst by 3D‐Printed Miniaturized Reactors

High temperature synthesis and treatments are ubiquitous in chemical reactions and material manufacturing. However, conventional sintering furnaces are bulky and inefficient with a narrow temperature range (<1500 K) and slow heating rates (<100 K min^?1), which are undesirable for many applications that require transient heating to produce ideal nanostructures. Herein, a 3D‐printed, miniaturized reactor featuring a dense micro‐grid design is developed to maximize the material contact and therefore acheive highly efficient and controllable heating. By 3D printing, a versatile, miniaturized reactor with microscale features can be constructed, which can reach a much wider temperature range (up to ≈3000 K) with ultrafast heating/cooling rates of ≈10⁴ K s^?1. To demonstrate the utility of the design, rapid and batch synthesis of Ru nanoparticles supported in ordered mesoporous carbon is performed by transient heating (1500 K, 500 ms). The resulting ultrafine and uniform Ru nanoparticles (≈2 nm) can serve as a cathode in Li‐CO₂ batteries with good cycling stability. The miniaturized reactor, with versatile shape design and highly controllable heating capabilities, provides a platform for nanocatalyst synthesis with localized and ultrafast heating toward high temperatures that is otherwise challenging to achieve.     

3D‐Printed Transparent Glass

Silica inks are developed, which may be 3D printed and thermally processed to produce optically transparent glass structures with sub‐millimeter features in forms ranging from scaffolds to monoliths. The inks are composed of silica powder suspended in a liquid and are printed using direct ink writing. The printed structures are then dried and sintered at temperatures well below the silica melting point to form amorphous, solid, transparent glass structures. This technique enables the mold‐free formation of transparent glass structures previously inaccessible using conventional glass fabrication processes.     

3D‐Printed,All‐in‐One Evaporator for High‐Efficiency Solar Steam Generation under 1 Sun Illumination

Using solar energy to generate steam is a clean and sustainable approach to addressing the issue of water shortage. The current challenge for solar steam generation is to develop easy‐to‐manufacture and scalable methods which can convert solar irradiation into exploitable thermal energy with high efficiency. Although various material and structure designs have been reported, high efficiency in solar steam generation usually can be achieved only at concentrated solar illumination. For the first time, 3D printing to construct an all‐in‐one evaporator with a concave structure for high‐efficiency solar steam generation under 1 sun illumination is used. The solar‐steam‐generation device has a high porosity (97.3%) and efficient broadband solar absorption (>97%). The 3D‐printed porous evaporator with intrinsic low thermal conductivity enables heat localization and effectively alleviates thermal dissipation to the bulk water. As a result, the 3D‐printed evaporator has a high solar steam efficiency of 85.6% under 1 sun illumination (1 kW m^?2), which is among the best compared with other reported evaporators. The all‐in‐one structure design using the advanced 3D printing fabrication technique offers a new approach to solar energy harvesting for high‐efficiency steam generation.     

Conductivity Maximum in 3D Graphene Foams

In conventional foams, electrical properties often play a secondary role. However, this scenario becomes different for 3D graphene foams (GrFs). In fact, one of the motivations for synthesizing 3D GrFs is to inherit the remarkable electrical properties of individual graphene sheets. Despite immense experimental efforts to study and improve the electrical properties of 3D GrFs, lack of theoretical studies and understanding limits further progress. The causes to this embarrassing situation are identified as the multiple freedoms introduced by graphene sheets and multiscale nature of this problem. In this article, combined with transport modeling and coarse‐grained molecular dynamic (MD) simulations, a theoretical framework is established to systematically study the electrical conducting properties of 3D GrFs with or without deformation. In particular, through large‐scale and massive calculations, a general relation between contact area and conductance for two van der Waals bonded graphene sheets is demonstrated, in terms of which the conductivity maximum phenomenon in GrFs is first theoretically proposed and its competition mechanism is explained. Moreover, the theoretical prediction is consistent with previous experimental observations.     

3D‐Printed Scanning‐Probe Microscopes with Integrated Optical Actuation and Read‐Out

Scanning‐probe microscopy (SPM) is the method of choice for high‐resolution imaging of surfaces in science and industry. However, SPM systems are still considered as rather complex and costly scientific instruments, realized by delicate combinations of microscopic cantilevers, nanoscopic tips, and macroscopic read‐out units that require high‐precision alignment prior to use. This study introduces a concept of ultra‐compact SPM engines that combine cantilevers, tips, and a wide variety of actuator and read‐out elements into one single monolithic structure. The devices are fabricated by multiphoton laser lithography as it is a particularly flexible and accurate additive nanofabrication technique. The resulting SPM engines are operated by optical actuation and read‐out without manual alignment of individual components. The viability of the concept is demonstrated in a series of experiments that range from atomic‐force microscopy engines offering atomic step height resolution, their operation in fluids, and to 3D printed scanning near‐field optical microscopy. The presented approach is amenable to wafer‐scale mass fabrication of SPM arrays and capable to unlock a wide range of novel applications that are inaccessible by current approaches to build SPMs.