Abstract

ABSTRACTThe need to reduce the energy consumed and the carbon footprint generated by firing ceramics has stimulated research to develop consolidation techniques operating at lower temperatures, ideally not exceeding 300 °C. This has been realised in Ultra Low Energy Sintering (ULES) using high pressure (hundreds of MPa) in the presence of a transient liquid phase, which accelerates plasticity, grain boundary/surface diffusion and mass transport. Several ULES techniques have been developed in the past 50 years, and a common feature of all of them is low temperature consolidation, through mechanisms not yet fully understood, enabling multi-material integration (e.g. organics and inorganics). This research could transform the traditional firing of functional and structural materials. Early stage work on ULES, started in the 1960s, clearly demonstrated cohesion between the compacted particles exceeding what was possible if simply produced by Van der Waals bonding, suggesting the formation of primary inter-particle bonds. Surprisingly, metals Cold Sintered (CS) in dry conditions at room temperature can be even stronger than their counterparts sintered at high temperatures (typically ≈ 2/3 Tm). Hydrothermal Hot Pressing (HHP) was originally conceived in the context of sustainability and environmental preservation, with some examples being the concept of ‘synthetic rock’ for immobilisation of toxic/radioactive waste and the consolidation of high surface area porous ceramics for filtration. Follow up work on HHP considered the possibility of recreating in the lab bio-mineralisation using hydroxyapatite and bioglass (including hybrids) as proof of concept. Recent work on the Cold Sintering Process has demonstrated the potential to bridge the processing gap of multi-material devices (sensors, batteries, 5G antennas, electronic components and biomaterials), enabling integration of polymers, ceramics and metals without degradation of the individual components both at the bulk and interface level. The absence of heating unlocks grain boundary design to an unprecedented level, offering further degrees of freedom in tuning functional properties.This review provides a wide perspective on room temperature consolidation, and covers the related but fragmented work published (≈ 450 papers) during the past 50 years, encompassing the relevant work developed in different disciplines including chemistry, physics, biology and geoscience. Liquid-assisted or liquid-mediated phenomena involving diffusion, plasticity, rheology, and grain growth are still largely unexplored in material science. The purpose of bringing together this literature is to build a general and multidisciplinary knowledge to guide future research directions. Both the reduction of energy consumption and carbon footprint are driving the growing interest in ULES, which could reinvent the concept of sintering, ‘rendering kilns obsolete’. Also, ULES has the potential to produce new classes of materials that cannot be fabricated using conventional routes.

Highlights

  • Most ceramics are prepared using green forming followed by firing, which is a highly energy intensive process involving temperatures usually above 1000 °C

  • Since the process involves the use of pressure, comparative analysis between reactive Hydrothermal Liquid Phase Sintering (rHLPS) and Hydrothermal Hot Pressing (HHP) could help to decouple the effects of chemical reactions from consolidation; this could pave the way for hybrid techniques where the compacting uniaxial pressure is for example applied after a hydrothermal reaction reaches completion

  • Ultra Low Energy Sintering (ULES) could replicate biomineralisation and lithification processes, which are the greenest way of producing ceramics and their composites

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Summary

Introduction

Most ceramics are prepared using green forming followed by firing, which is a highly energy intensive process involving temperatures usually above 1000 °C. Since sintering is a process driven by reduction of surface energy, a possible way to reduce energy consumption might involve selective heating of the surface of the particles. Taking inspiration from inorganic materials produced in nature, there are plenty of everyday examples of inorganic materials formed at room temperature without the need of additional heat. These include sedimentary rocks produced by lithification (literally, the process of turning particles into stone), stalactites from precipitation of minerals from mineralised water dripping through cave ceilings, bones/teeth from bio-mineralisation, construction of buildings from cementation and spicules (sea sponges) from the polycondensation of silicic acid. Predict a processing window (i.e. pressure, type and amount of liquid, setups and temperature) for different materials based on their ionic, metallic or covalent bonding

Historical perspective
Overview of ULES processes
Cold Sintering in dry condition: materials and applications
Early stage
Hydrothermal hot pressing According to
Reactive hydrothermal liquid phase sintering
Pressure-less wet ULES and 3D shaping Professor Jantunen’s group at the
Cold sintering process (Randall’s method) The CSP was developed at Pennsylvania
Formation of inter-particle primary bond in ULES
Theory of sintering applied to ULES
Findings
Conclusions and future trends
Full Text
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