ConspectusThe field of two-dimensional (2D) carbides and nitrides (MXenes) has increased by leaps and bounds since the isolation of Ti3C2Tx, the first MXene, in 2011. MXenes offer high specific surface area and a unique electronic structure leading to properties with a broad potential of applications. For instance, MXenes as heterogeneous catalysts may constitute a strategic response to the challenge posed by the scarcity and elevated costs of noble metals involved in many industrial catalysts. In fact, the exploration of MXenes in heterogeneous catalysis has opened new avenues for the application of these materials, expanding their role beyond traditional material applications. This Account focuses on the exploration of MXenes as catalysts for the capture and conversion of CO2 from a computational materials science perspective. It systematically reviews our contributions in first-principles modeling going beyond the standard extended surface models. It starts by briefly discussing the kinetic phase diagrams as a useful tool to predict the practical conditions for CO2 activation by on MXenes. The ease of CO2 activation and dissociation on MXenes makes them feasible catalysts for CO2 conversion, for instance through the reverse water gas shift reaction. Progresses in this direction are discussed in this Account including key aspects affecting the catalytic performance of MXenes revealed by multiscale, mean-field kinetic, and kinetic Monte Carlo simulations. Overall, our computational strategy combining first-principles calculations, kinetic phase diagrams, and multiscale modeling provides a workflow to scrutinize the catalytic capability of new MXenes, shedding light into the predicted behavior, ultimately providing rational structure–property relationships which drive experimentalists toward the best possible candidates.

ConspectusThe self-assembly of inorganic nanoparticles (NPs) endows the resulting assembles with unique collective optical, electrical, and magnetic properties beyond the individual NPs. Nanoscale colloidal molecules (CMs) and colloidal polymers (CPs), which use NPs as building blocks to mimic the structural features of conventional molecules and polymers, have attracted significant attention due to their extraordinary collective properties, making them promising candidates for applications in sensing, catalysis, electronics, photonics, and energy harvesting. However, achieving precise nanoscale assembly of NPs into well-defined architectures such as CMs and CPs remains challenging. Polymer-grafted NPs (PGNPs), also known as hairy NPs, offer a versatile and practical platform for constructing such assemblies due to their hybrid organic–inorganic nature. More importantly, polymers used as surface ligands offer several key advantages: (i) they provide a wide range of interactions, tunable responsiveness, and excellent biocompatibility; (ii) their size is comparable to that of NPs, providing improved control over the NP assembly; (iii) their long, flexible chains enhance the colloidal stability of both individual NPs and their assemblies; and (iv) their intrinsic self-assemble behavior can enrich complexity and diversity of the final assemblies. Despite these benefits, challenges remain in developing precise and controllable strategies for assembling PGNPs into well-defined CMs and CPs, as well as in fully understanding the underlying formation mechanisms.In this Account, we summarize recent advances in the design and fabrication of CMs and CPs by employing PGNPs as building blocks. We begin by outlining the conformational behaviors of polymers capped on the NP surfaces and the three typical synthetic approaches for PGNPs: “grafting to”, “grafting from”, and one-pot synthesis. In the second section, we present the directional self-assembly of spherical PGNPs into CMs and CPs, with emphasis on the manipulation of interparticle interactions, including chemical reaction-induced recognitive interaction, electrostatic interaction, hydrogen bonding, and halogen bonding. The third section focuses on shape-anisotropic PGNPs and their unique self-assemble behavior. In the fourth section, we discuss the formation mechanisms of these assemblies with the assist of the time-dependent experimental studies and computational simulations. The fifth section highlights strategies for preparing plasmonic CM superlattices and discuss their emerging collective properties. Finally, we discuss the current challenges in this field and offer perspectives on future research directions.

ConspectusCancer, responsible for approximately 16.8% of global mortality, remains one of the most formidable challenges to public health. Chemotherapy remains a mainstay of cancer treatment, utilizing small-molecule agents to inhibit tumor growth, invasion, and metastasis. Camptothecin (CPT) exhibits broad-spectrum antitumor activity; however, its clinical potential is severely limited by poor aqueous solubility, low stability, and insufficient tumor selectivity, which collectively restrict its bioavailability and therapeutic efficacy. Conventional formulations such as covalent chemical modifications, lipid encapsulations and PEGylated conjugates have been developed to address these issues but often suffer from short half-lives, low drug-loading capacities (<20%), instability under physiological conditions, and inadequate tumor accumulation.Inspired by natural self-assembly processes exemplified by DNA and collagen, supramolecular chemistry offers a versatile approach to constructing dynamic, programmable architectures through noncovalent interactions. These systems mimic biological organization and enable tunable functionalities for drug delivery, tissue regeneration, and immune modulation. Over the past decade, our group has established an approach that precisely controls supramolecular self-assembly and chiral nanostructure formation through the elucidation of how specific noncovalent interactions govern assembly dynamics, thereby transforming supramolecular chemistry into a programmable platform for diverse biomedical applications such as biocatalysis, regenerative medicine, and cancer therapy. All the results have demonstrated the superiority of supramolecular chiral nanofiber structures in biofields. Expanding on this groundwork, we have successfully transformed CPT from a conventional small-molecule chemotherapeutic into a supramolecular chiral nanofibers’ therapeutic platform. Through a straightforward self-assembly strategy driven by noncovalent interactions, CPT molecules can spontaneously self-assemble into controllable helical nanofibers without the need for additional chemical modification. The obtained dynamic self-assemblies exhibit improved stability, high drug loading, and efficient tumor penetration by targeting the mitochondria, achieving precise subcellular localization and robust induction of immunogenic cell death, thus representing a minimalist yet powerful approach to supramolecular cancer therapy.This Account highlights our group’s recent advances in chiral supramolecular materials for cancer therapy, which have pioneered a supramolecular engineering approach for CPT-based treatment. We first discuss the design of responsive nanostructures that exploit physical stimuli within the tumor microenvironment (TME) for controlled drug release. Subsequently, we delve into the novel strategy of chirality-driven tumor immunotherapy. A specific focus is placed on potent chiral supramolecular assemblies, particularly CPT-based nanofibers, which exemplify this immunotherapeutic approach. Following the discussion of these scientific breakthroughs, we address the critical challenges in translating such supramolecular materials from the laboratory to clinical trials. It is hoped that the insights provided here will serve as a valuable foundation for integrating supramolecular engineering with translational oncology, thereby paving the way toward precision supramolecular therapeutics.

ConspectusAs sustainability becomes a driving force in chemical research, designing hybrid materials that combine renewable organic matter with functional inorganic components has taken center stage. Among potential bio-based feedstocks, lignin stands out due to its abundance, chemical diversity, and renewable origin. Produced industrially as a pulp and paper byproduct, this complex polyphenol is the most abundant natural source of aromatic carbon. Lignin’s structural complexity, arising from a random polymerization of guaiacyl, syringyl, and p-hydroxyphenyl units, endows it with rich functionality but also poses challenges in achieving reproducibility and material consistency. Despite these barriers, lignin’s greatest potential may lie in its role as a molecularly active component at hybrid interfaces. Its phenolic hydroxyls, methoxy groups, and carboxylic functionalities support a range of interactions with inorganic phases, including hydrogen bonding, π–π stacking, electrostatics, and metal coordination. These interfacial chemistries allow lignin to serve as a support or stabilizer and actively modulate charge dynamics and interfacial behavior in functional materials. In this Account, we focus on how molecular-level interface design can take advantage of lignin’s potential for sustainable applications in photo- and electrocatalysis and in tribology, which are fields deeply tied to environmental remediation and energy efficiency. We present strategies ranging from hydroxymethylation for nanoparticle assembly to electrochemical depolymerization, all aimed at optimizing lignin’s structure and reactivity for hybrid systems. In photocatalysis, lignin–Bi4O5Br2/BiOBr nanocomposites enhance visible-light-driven hydrogen peroxide (H2O2) production from seawater. These materials leverage lignin’s redox-active groups to facilitate charge separation and oxygen reduction, while improving stability under saline conditions. In tribology, hydroxymethylated lignin nanoparticles (HLNPs) act as scaffolds for MoS2 nanoflowers, preventing aggregation and enabling stable dispersion as a bioderived additive in lubricants. The resulting hybrids deliver significant reductions in wear and friction, outperforming both lignin-only and MoS2-only systems. Here, lignin contributes both dispersion control and interfacial mechanical functionality. We further highlight the valorization of sugar-cane-derived lignin through the synthesis of nickel nanoparticle (NiNP)-decorated lignin biochar. Starting from waste bagasse, lignin is extracted, treated with Ni(NO3)2, and thermally converted to NiNP-decorated lignin biochar. When coated on carbon paper, this material acts as an efficient electrocatalyst for the depolymerization of lignin itself, forming a closed-loop system where lignin both forms and fuels its own transformation. The nanostructured carbon matrix stabilizes active Ni sites and supports effective charge transfer. Looking forward, standardization of lignin sources, integration of computational modeling and machine learning to guide interface engineering, and implementation of life-cycle assessments will be key to ensuring environmental benefit and reproducibility. Equally important is the adoption of operando spectroscopic techniques capable of tracking interface evolution under realistic working conditions, which will be essential for decoding structure–function relationships. Across these case studies, a recurring design principle emerges: lignin not only provides structural support or dispersion but also contributes actively to interfacial charge redistribution and mechanical stabilization. By recognizing lignin as a redox-active and mechanically cooperative component, rather than a passive scaffold, we open a generalizable route to designing sustainable hybrid materials whose function is rooted in their interfacial chemistry.

ConspectusPlastic pollution and climate change are interconnected global environmental challenges. Conventional methods (incineration and landfills) exacerbate these issues by emitting greenhouse gases and releasing micro/nanoplastics. To simultaneously address these two critical environmental issues, we upcycle plastic waste into porous carbon materials, enabling high-performance postcombustion CO2 capture in a transformative and practical manner. This strategy tackles environmental pollution, aligns with circular economy principles, and supports several of UN Sustainable Development Goals (SDGs). We conduct systematic studies, including experimental validations, numerical simulations, and machine learning (ML)-empowered optimizations, to provide detailed guidelines for upcycling plastic waste into porous carbons with high-performance CO2 capture.Synthesis routes vary in their environmental benefits and economic feasibility. Different activating agents (e.g., steam, potassium hydroxide, and urea) are comprehensively compared. Experimental operating parameters (e.g., activation temperature, activating agent type, and loading mass ratio) are optimized to produce micropore-dominated carbon materials that exhibit excellent CO2 adsorption performance. Our main results show that plastic-derived porous carbons achieved high specific surface areas (up to 2,060 m2/g) and micropore volumes (∼1.02 cm3/g), demonstrating great potential in CO2 adsorption capture. Functional groups like C═O and O–H further enhance the CO2 adsorption capacity due to their strong dipole–quadrupole interactions with CO2 molecules and the formation of hydrogen bonding. Based on experimental investigations, Grand Canonical Monte Carlo (GCMC) simulations reveal that narrow micropores (<0.8 nm) and optimal isosteric heat (23–28 kJ/mol) favor CO2 physisorption.In this work, interpretable ML techniques, such as feature importance ranking and SHAP analysis, reveal the key structural and chemical features that dominate CO2 uptake performance. These include the pore size distribution and surface chemistry, which provide valuable guidance for the rational design of plastic-derived porous carbons. Building on these insights, we also apply ML, particularly active learning and particle swarm optimization (PSO) approaches, for iteratively identifying optimal synthesis parameters, thereby enhancing CO2 adsorption capacity by up to 2-fold relative to seed experiments. This strategy offers a more efficient route to performance improvement compared to conventional trial-and-error approaches.To ensure industrial applicability, we assess the cyclic performance of CO2 capture by temperature swing adsorption (TSA), pressure swing adsorption (PSA), and vacuum swing adsorption (VSA) processes and then scale these technical routes via process simulations. Multiobjective optimization achieves an excellent 35.13% exergy efficiency, aided by artificial neural network (ANN)-based surrogate modeling and genetic algorithms. This work was also studied from perspectives of both environmental benefits and economic feasibility to explore its potential for enabling sustainable development. This holistic and multidisciplinary strategy, combining materials science, AI algorithms, and environmental engineering, offers a carbon-negative and economically viable path to simultaneously mitigate climate change and achieve a circular plastic economy. Our future work will focus on data set expansions, intelligent optimizations, and large-scale deployment for real-world impacts.

ConspectusThe rapid advancement of electronic and electrical equipment has played a pivotal role in driving global economic growth, becoming indispensable to modern society. However, as equipment becomes increasingly miniaturized and highly integrated, the associated thermal management challenges have escalated. In addition, the occurrence of more frequent and intense heatwaves, driven by climate change, has compounded these challenges, making overheating a critical issue. When electronic and electrical devices overheat, their performance degrades, and their lifespan shortens, leading to potential failures and increased maintenance costs. To combat overheating, active cooling systems such as air and liquid cooling are commonly used. While effective, these systems are energy-intensive and require substantial power to operate. This increased energy consumption places pressure on global energy resources and contributes to environmental concerns, particularly regarding carbon emissions. Passive cooling materials, however, provide a promising solution, offering heat dissipation without consuming additional energy. This energy efficiency is especially important in the context of global sustainability goals.Passive cooling materials can be classified into three main categories: radiative cooling materials, sorption-based evaporative cooling materials, and hybrid passive cooling materials. Radiative cooling materials work by emitting heat into space through thermal radiation while reflecting sunlight to reduce heat absorption. This mechanism allows them to perform effectively even under high ambient temperatures and intense sunlight. Sorption-based evaporative cooling materials absorb heat through water desorption, offering significant cooling power and the ability to regenerate continuously without external energy input. These materials are particularly beneficial for applications in high-humidity regions. Hybrid passive cooling materials combine the benefits of radiative and sorption-based evaporative cooling, achieving superior cooling performance. This dual mechanism significantly enhances heat dissipation, offering many times the cooling power of radiative materials alone and making them ideal for high heat-generating electronics.This Account provides an in-depth exploration of these three categories of passive cooling materials, with a focus on their practical applications in electronic and electrical equipment. We begin by examining the fundamental principles of radiative cooling, emphasizing the critical material requirements, such as thermal conductivity, which enable effective heat dissipation above ambient temperatures. We will also highlight several successful applications of radiative cooling materials, including promising radiative cooling coatings. Additionally, we will discuss the principles of sorption-based evaporative cooling, comparing various sorbents and exploring innovative methods for preparing stable composites. Lastly, we will examine the principles of hybrid passive cooling materials and outline strategies for achieving high cooling power, along with an overview of promising materials for heat dissipation. In conclusion, we provide a forward-looking perspective on the development of passive cooling materials and their potential to address the evolving thermal management needs of electronic and electrical equipment.

CONSPECTUS: Skin electronics integrated with the human body have attracted significant global interest due to their potential applications in healthcare monitoring and motion sensing.Over the past few decades, electronic devices have become increasingly soft and stretchable with the progress of engineering and materials science, aiming to achieve enhanced integration with the skin and improved acquisition of physiological signals.However, owing to the delicate nature of human skin and its intricate role in regulating body temperature and fluid balance, electronic devices at the skin interface must not only exhibit mechanical compliance but also ensure physiological comfort.They should not block skin metabolism or cause skin damage during daily or long-term use.As a result, the materials used should be biocompatible with the skin/organs without leading to allergic reactions or inflammatory responses.Additionally, these materials should be readily processed into various formats to accommodate skin deformation and breath.As a natural biomaterial, silk is widely acknowledged as the ideal material for developing skin-friendly electronics due to its multifaceted benefits in comparison with many synthetic polymers, including good biocompatibility, tailorable biodegradability, and versatile processability.These properties, which are linked to the conformation of silk, grant silk materials the capacity to be programmed as soft and stretchable as skin.Furthermore, silk can be processed through various manufacturing techniques, resulting in diverse material formats like fibers, mats, thin films, hydrogels, and scaffolds that are readily attainable.These rich silk formats exhibit diverse properties and performance characteristics, making them suitable for meeting various requirements in both in vivo and in vitro applications.Leveraging these attributes, natural and regenerated silk materials have been successfully employed in skin-integrated electronics, including but not limited to textile electronics, transient biosensors, adhesive ionic gels, conformal/breathable/stretchable electrodes, and smart dressings.These electronic devices show a high degree of geometric and mechanical compatibility with the skin, and more importantly, they do not cause physical discomfort or disturb skin functions, providing novel prospects for developing high-performance and biologically compliant skin electronics.In this Account, we highlight recent progress of silk-based materials for skin electronics that prioritize both mechanical and biological compliance.We begin with a comprehensive exploration of the hierarchical structures and inherent properties of natural silk fibers, showing the biocompatibility and biodegradability of silk adapted for bioelectronics, as well as the solution-processability facilitated for the creation of silk materials with versatile formats and properties.Subsequently, we systematically discuss the design and functionality of silk-based skin electronics through engineering structures and materials to fulfill the requirements of high mechanical and biological compliance with the skin.Finally, we elucidate the limitations of current silk-based skin electronics and briefly envision the future challenges and prospects for developing silk as high-performance electronics for comfortable wearing systems.