Hierarchical zeolites combine the intrinsic catalytic properties of microporous zeolites and the enhanced access and transport of the additional meso- and/or macroporous system. These materials are the most desirable catalysts and sorbents for industry and become a highly evolving field of important current interests. In addition to the enhanced mass transfer leading to high activity, selectivity, and cycle time, another essential merit of the hierarchical structure in zeolite materials is that it can significantly improve the utilization effectiveness of zeolite materials resulting in the minimum energy, time, and raw materials consumption. Substantial progress has been made in the synthesis, characterization, and application of hierarchical zeolites. Herein, we provide an overview of recent achievements in the field, highlighting the significant progress in the past decade on the development of novel and remarkable strategies to create an additional pore system in zeolites. The most innovative synthesis approaches are reviewed according to the principle, versatility, effectiveness, and degree of reality while establishing a firm link between the preparation route and the resultant hierarchical pore quality in zeolites. Zeolites with different hierarchically porous structures, i.e., micro-mesoporous structure, micro-macroporous structure, and micro-meso-macroporous structure, are then analyzed in detail with concrete examples to illustrate their benefits and their fabrications. The significantly improved performances in catalytic, environmental, and biological applications resulting from enhanced mass transport properties are discussed through a series of representative cases. In the concluding part, we envision the emergence of "material-properties-by-quantitative and real rational design" based on the "generalized Murray's Law" that enables the predictable and controlled productions of bioinspired hierarchically structured zeolites. This Review is expected to attract important interests from catalysis, separation, environment, advanced materials, and chemical engineering fields as well as biomedicine for artificial organ and drug delivery systems.

Hierarchically Structured Zeolites: From Design to Application.

An increasing utilization of flexible healthcare electronics and biomedicine-related therapeutic materials urges the development of multifunctional wearable/flexible smart fabrics for personal therapy and health management. However, it is currently a challenge to fabricate multifunctional and on-body healthcare electronic devices with reliable mechanical flexibility, excellent breathability, and self-controllable joule heating effects. Here, we fabricate a multifunctional MXene-based smart fabric by depositing 2D Ti3C2Tx nanosheets onto cellulose fiber nonwoven fabric via special MXene-cellulose fiber interactions. Such multifunctional fabrics exhibit sensitive and reversible humidity response upon H2O-induced swelling/contraction of channels between the MXene interlayers, enabling wearable respiration monitoring application. Besides, it can also serve as a low-voltage thermotherapy platform due to its fast and stable electro-thermal response. Interestingly, water molecular extraction induces electrical response upon heating, i.e., functioning as a temperature alarm, which allows for real-time temperature monitoring for thermotherapy platform without low-temperature burn risk. Furthermore, metal-like conductivity of MXene renders the fabric an excellent Joule heating effect, which can moderately kill bacteria surrounding the wound in bacteria-infected wound healing therapy. This work introduces a multifunctional smart flexible fabric suitable for next-generation wearable electronic devices for mobile healthcare and personal medical therapy.

Smart Ti3C2Tx MXene Fabric with Fast Humidity Response and Joule Heating for Healthcare and Medical Therapy Applications

DOI: 10.1002/aenm.201903921 us warm in cold climates and shielded us from the nakedness for modesty and civilization.[1,2] Cloth is also a platform for artists, designers, and tailors to advance the clothing demands with emerging materials, process, and fashion.[2] While the majority of the functionalities of clothes lie in their physical attributes, such as their softness, breathability, air/ vapor permeability, and, of course the appearance, their role in thermal management is equally, if not more, important. The primary goal of clothing is to satisfy human being’s basic needs in thermal comfort, by providing cooling in the hot environment or heating in the cold environment.[1] The energy management aspect of clothing is becoming an increasingly important and attractive aspect due to our increasing awareness to energy consumption and our persisting pursuit of comfort and health. The finite availability and the associated environmental consequence of fossil fuels have motivated us to save energy from virtually all aspects of our daily lives. A suitable thermal envelop is a necessity for our living and working. To create a comfortable indoor environment, the building heating, ventilation, and air conditioning (HVAC) systems are widely used for space cooling and heating at the expense of excessive energy consumption.[3–6] According to United States In this decade, the demands of energy saving and diverse personal thermoregulation requirements along with the emergence of wearable electronics and smart textiles give rise to the resurgence of personal thermal management (PTM) technologies. PTM, including personal cooling, heating, insulation, and thermoregulation, are far more flexible and extensive than the traditional air/liquid cooling garments for the human body. Concomitantly, many new advanced materials and strategies have emerged in this decade, promoting the thermoregulation performance and the wearing comfort of PTM simultaneously. In this review, an overview is presented of the state-ofthe-art and the prospects in this burgeoning field. The emerging materials and strategies of PTM are introduced, and classed by their thermal functions. The concept of infrared-transparent visible-opaque fabric (ITVOF) is first highlighted, as it triggers the work on advanced PTM by combining it with radiative cooling, and the corresponding implementations and realizations are subsequently introduced, followed by wearable heaters, flexible thermoelectric devices, and sweat-management Janus textiles. Finally, critical considerations on the challenges and opportunities of PTM are presented and future directions are identified, including thermally conductive polymers and fibers, physiological/psychological statistical analysis, and smart PTM strategies.

Emerging Materials and Strategies for Personal Thermal Management

Excessive sweat secreted from the skin often causes undesired adhesion from wetted textiles and cold sensations. Traditional hydrophilic textiles such as cotton can absorb sweat but retain it. A hydrophobic/superhydrophilic Janus polyester/nitrocellulose textile embedded with a conical micropore array with a hydrophilic inner surface that can achieve directional liquid transport (with an ultrahigh directional water transport capability of 1246%) and maintain human body temperature (2-3 °C higher than with cotton textiles) is demonstrated. When the hydrophobic polyester layer with large opening of hydrophilic conical micropores contacts the liquid, the Janus polyester/nitrocellulose textile can pump it to the superhydrophilic nitrocellulose layer through the hydrophilic conical micropores driven by capillary force. The Janus polyester/nitrocellulose textile can weaken undesired wet adhesion and heat loss due to the removal of liquid. The water wicking and air permeability of the Janus polyester/nitrocellulose textile is comparable to those of traditional cloths. This study is valuable for designing of functional textiles with directional water transport properties for personal drying and warming applications.

Bioinspired Janus Textile with Conical Micropores for Human Body Moisture and Thermal Management

Frequent oil spills and the ever-growing discharge of industrial oily wastewater seriously threaten ecosystems and human safety and result in huge economic loss, which has stimulated researchers to explore advanced oil/water separation materials. Electrospun nanofibrous membranes, featuring tunable wettability, good flexibility, high porosity, and outstanding pore connectivity, have received increasing attention. In this review, we aim to present the design and fabrication of electrospun flexible nanofibrous membranes with special wettability for oil/water separation. This review focuses on the discussion of various electrospun flexible membranes, assorted into three categories, including polymer-based membranes, ceramic-based membranes, and carbon-based membranes. In each type, the representative studies, fabrication techniques, and the synergistic effect among the membrane structure, selective wettability, and oil/water separation performance are discussed in detail. Finally, future perspectives and challenges in this promising field are highlighted.

Electrospun flexible nanofibrous membranes for oil/water separation

Directional water transport is a predominant part of functional textiles used for continuous sweat release in daily life. However, it has remained a great challenge to design such textiles which ensure continuous directional water transport and superior prevention of water penetration in the reverse direction. Here, a scalable strategy is reported to create trilayered fibrous membranes with progressive wettability by introducing a transfer layer, which can guide the directional water transport continuously and spontaneously, thus preventing the skin from being rewetted. The resulting trilayered fibrous membranes exhibit a high one-way transport index R (1021%) and a desired breakthrough pressure (16.1 cm H2 O) in the reverse direction, indicating an ultrahigh directional water transport capacity. Moreover, on the basis of water transport behavior, a plausible mechanism is proposed to provide insight into the integrative and cooperative driving forces at the interfaces of trilayered hydrophobic/transfer/superhydrophilic fibrous membranes. The successful synthesis of such fascinating materials would be valuable for the design of functional textiles with directional water transport properties for personal drying applications.

Continuous, Spontaneous, and Directional Water Transport in the Trilayered Fibrous Membranes for Functional Moisture Wicking Textiles

Both antigravity directional water transport and ultrafast evaporation are critical to achieving a high-performance moisture-wicking fabric. The transpiration in vascular plants possess both of these features, which is due to their optimized hierarchical structure composed of multibranching porous networks following Murray's law. However, it remains a great challenge to simultaneously realize the ultrafast water transport and evaporation by mimicking nature's Murray networks in the synthetic materials. Here, we report a synergistic assembly strategy to create a biomimetic micro- and nanofibrous membrane with antigravity directional water transport and quick-dry performance by combining a multibranching porous structure and surface energy gradient, overcoming previous limitations. The resulting fiber-based porous Murray membranes exhibit an ultrahigh one-way transport capability ( R) of 1245%, a desired overall moisture management capability (OMMC) of 0.94, and an outstanding water evaporation rate of 0.67 g h-1 (5.8 and 2.1 times higher than the cotton fabric and Coolmax fabric, respectively). Overall, the successful synthesis of these biomimetic porous Murray membranes should serve as a source of inspiration for the development of moisture-wicking technologies, providing personal comfort in hot or humid environments.

Zhan Huang

Papers

Continuous, Spontaneous, and Directional Water Transport in the Trilayered Fibrous Membranes for Functional Moisture Wicking Textiles

Biomimetic Fibrous Murray Membranes with Ultrafast Water Transport and Evaporation for Smart Moisture-Wicking Fabrics.