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Skin-mountable capacitive-type strain sensors with great linearity and low hysteresis provide inspiration for the interactions between human and machine. For practicality, high sensing performance, large stretchability, and self-healing are demanded but limited by stretchable electrode and dielectric and interfacial compatibility. Here, we demonstrate an extremely stretchable and self-healing conductor via both hard and soft tactics that combine conductive nanowire assemblies with double dynamic network based on π-π attractions and Ag-S coordination bonds. The obtained conductor outperforms the reported stretchable conductors by delivering an elongation of 3250%, resistance change of 223% at 2000% strain, high durability, and multiresponsive self-healability. Especially, this conductor accommodates large strain of 1500% at extremely knotted and twisted deformations. By sandwiching hydrogel conductors with a newly developed dielectric, ultrahigh stretchability and omni-healability are simultaneously achieved for the first time for a capacitive strain sensor inspired by metal-thiolate coordination chemistry, showing great potentials in wearable electronics and soft robotics.

Two-dimensional (2D) IV–VI nanomaterials have been important candidates for energy conversion and storage. However, there is still lack of a simple method of realizing control synthesis of IV–VI na...

Self-healability is essential for supercapacitors to improve their reliability and lifespan when powering the electronics. However, the lack of a universal healing mechanism leads to low capacitive performance and unsatisfactory intelligence. Here, we demonstrate a multi-responsive healable supercapacitor with integrated configuration assembled from magnetic Fe3O4@Au/polyacrylamide (MFP) hydrogel-based electrodes and electrolyte and Ag nanowire films as current collectors. Beside a high mechanical strength, MFP hydrogel exhibits fast optical and magnetic healing properties arising from distinct photothermal and magneto-thermal triggered interfacial reconstructions. By growing electroactive polypyrrole nanoparticles into MFP framework as electrodes, the assembled supercapacitor exhibits triply-responsive healing performance under optical, electrical and magnetic stimuli. Notably, the device delivers a highest areal capacitance of 1264 mF cm−2 among the reported healable supercapacitors and restores ~ 90% of initial capacitances over ten healing cycles. These prominent performance advantages along with the facile device-assembly method make this emerging supercapacitor highly potential in the next-generation electronics., Self-healing property is important for supercapacitors when powering the electronics, but designing devices that possess a universal healing mechanism remains challenging. Here, the authors achieve an optically, electrically, and magnetically-responsive self-healing device with integrated configuration.

Conductive and adhesive hydrogels are promising materials for designing bioelectronics. To satisfy the high conductivity of bioelectronic devices, metal nanomaterials have been used to fabricate composite hydrogels. However, the fabrication of a conductive-nanomaterial-incorporated hydrogel with high performance is a great challenge because of the easy aggregation nature of conductive nanomaterials making processing difficult. Here, we report a kind of adhesive aero-hydrogel hybrid conductor (AAHC) with stretchable, adhesive and anti-bacteria properties by in situ formation of a hydrogel network in the aerogel-silver nanowires (AgNWs) assembly. The AgNWs with good conductivity are well-integrated on the inner-surface of shape-memory chitosan aerogel, which created a conductive framework to allow hydrogel back-filling. Reinforcement by the aerogel-silver makes the hybrid hydrogel tough and stretchable. Functional groups from the hydrogel allow strong adhesion to wet tissues through molecular stitches. The inherent bacteria-killing ability of silver ions endows the conductive hydrogel with excellent anti-bacteria performance. The proposed facile strategy of aerogel-assisted assembly of metal nanomaterials with hydrogel opens a new route to incorporate functional nanoscale building blocks into hydrogels.

We report that continuous MOF films with highly controlled thickness (from 44 to 5100 nm) can be deposited over length scales greater than 80 centimeters by a facile, fast, and cost-effective spray-coating method. Such success relies on our discovery of unprecedented perfectly dispersed colloidal solutions consisting of amorphous MOF nanoparticles, which we adopted as precursors that readily converted to the crystalline films upon low-temperature in situ heating. The colloidal solutions allow for the fabrication of compact and uniform MOF films on a great deal of substrates such as fluorine-doped tin oxide, glass, SiO2 , Al2 O3 , Si, Cu, and even flexible polycarbonate, widening their technological applications where substrates are essential. Despite the present work focuses on the fabrication of uniform cobalt-(2-methylimidazole)2 and zinc-(2-methylimidazole)2 films, our findings mark a great possibility in producing other high-quality MOF thin films on a large scale.

Introducing heating function to oil sorbents opens up a new pathway to the fast cleanup of viscous crude oil spills in situ. The oil sorption speed increases with the rise of the temperature, thus oil sorbents with high heating temperature are desirable. Besides, the oil sorbents also need to be produced environment-friendly. Here we present carbonized melamine-formaldehyde sponges (CMSs) that exhibited superior heating performance and the CMSs could be massively fabricated through a non-polluting pyrolysis process. The conductive CMSs could be heated over 300 °C with a low applied voltage of 6.9 V and keep above 250 °C for 30 min in the air without obvious damage. Such high heating performance enabled heating up the oil spills with a high rate of 2.65 °C·s−1 and 14% improvement of oil sorption coefficient compared with the state-of-the-art value. We demonstrated that one joule-heated CMS could continuously and selectively collect viscous oil spills (9,010 mPa·s) 690 times its own weight in one hour. The CMSs will be a highly competitive sorbent material for the fast remediation of future crude oil spills.

Siloxane rubber shows attractive properties of high stability, elasticity and transparency. Besides, the regulation of its properties renders it widely used in many application fields. However, most of the reported performance improvement methods of siloxane rubber focus on the change of chemical composition of siloxane rubber, including the design of molecular chain and the introduction of other compounds, etc. Such a strategy is still faced with many limitations in practical application. In this work, on the premise of not changing the chemical composition of siloxane rubber, we propose a facile solvothermal polymerization process to change the structure of cross-linking networks, so as to obtain the siloxane rubber with controllable mechanical properties. Compared to the normal curing method, we realized polydimethylsiloxane elastomer (PDMS) with maximum elongation of more than 3,000% (> 10 times of normally cured one) and tensile modulus lower than 0.15 MPa (< 1/10 of normally cured one). In addition to superior stretchability, it gains extra high softness, stickiness and sensitive response to organic solvents. Based on our solvothermal cured PDMS, its applications in oil collection and organic solvent sensor have been demonstrated. It is expected that this method can be readily utilized widely and shows great application potentials.

Biomimetic nacrelike designs not only present a rational strategy for preparing robust materials but also open the avenue for regulating nanofluidic ion transport.

Suppressing the polysulfide shuttle effect and promoting the conductivity of electrode materials have become efficient ways to achieve high cycling stability for Li–S batteries. However, this still remains a challenge. New multicore closely packed ultrathin-MnO2@N-doped carbon-gear yolk–shell micro-nanostructures are explored as the S host material to trap polysulfides and enhance conductivity. Such composites can accommodate S mass-loading up to 80 wt% via a valid sulfur solution infiltration approach. The cooperation of ultrathin-MnO2 yolks with N-doped carbon internal gear shells can well suppress the polysulfide shuttle effect by strong chemical interactions and physical confinement as well as enhanced conductivity for excellent Li–S battery properties, which enable an initial gravimetric capacity of 1245 mA h g−1 and a low decay rate of 0.03% per cycle over 1000 cycles at 1C. In particular, the composite delivers an initial gravimetric capacity of 1097.8 mA h g−1 and volumetric capacity of 1059.6 mA h cm−3 at 2C rate. Specifically, the electrochemical performance of the designed composite at different electrolyte/S ratios is firstly investigated in this study, and is a promising approach with the high-performance cathode material for Li–S batteries.

Undoubtedly humidity is a non-negligible and sensitive problem for cellulose, which is usually regarded as one disadvantage to cellulose-based materials because of the uncontrolled deformation and mechanical decline. But the lack of an in-depth understanding of the interfacial behavior of nanocellulose in particular makes it challenging to maintain anticipated performance for cellulose-based materials under varied relative humidity (RH). Starting from multiscale mechanics, we herein carry out first-principles calculations and large-scale molecular dynamics simulations to demonstrate the humidity-mediated interface in hierarchical cellulose nanocrystals (CNCs) and associated deformation modes. More intriguingly, the simulations and subsequent experiments reveal that water molecules (moisture) as the interfacial media can strengthen and toughen nanocellulose simultaneously within a suitable range of RH. From the perspective of interfacial design in materials, the anomalous mechanical behavior of nanocellulose with humidity-mediated interfaces indicates that flexible hydrogen bonds (HBs) play a pivotal role in the interfacial sliding. The difference between CNC-CNC HBs and CNC-water-CNC HBs triggers the humidity-mediated interfacial slipping in nanocellulose, resulting in the arising of a pronounced strain hardening stage and the suppression of strain localization during uniaxial tension. This inelastic deformation of nanocellulose with humidity-mediated interfaces is similar to the Velcro-like behavior of a wet wood cell wall. Our investigations give evidence that the humidity-mediated interface can promote the mechanical enhancement of nanocellulose, which would provide a promising strategy for the bottom-up design of cellulose-based materials with tailored mechanical properties.

Lightweight yet strong paper with high toughness is desirable especially for impact protection. Herein we demonstrated electrically conductive and mechanically robust paper (AP/PB-GP) made of reduced graphene oxide via interfacial crosslinking with 1-aminopyrene (AP) and 1-pyrenebutyrat (PB) small molecules. The AP/PB-GP with thickness of over ten micrometer delivers a record-high toughness (∼69.67 ± 15.3 MJ m−3 in average), simultaneously with superior strength (close to 1 GPa), allowing an impressive specific penetration energy absorption (∼0.17 MJ kg−1) at high impact velocities when used for ballistic impact protection. Detailed interfacial and structural analysis reveals that the reinforcement is synergistically determined by π-π interaction and H-bonding linkage between adjacent graphene lamellae. Especially, the defective pores within the graphene platelets benefit the favorable adsorption of the pyrene-containing molecules, which imperatively maximizes the interfacial binding, facilitating deflecting crack and plastic deformation under loading. Density functional theory simulation suggests that the coupling between the polar functional groups, e.g., −COOH, at the edges of graphene platelets and −NH2 and −COOH of AP/PB are critical to the formation of hydrogen bonding network.

Magnesium calcite (Mg-calcite) mesocrystal is widespread in the biominerals with specific functions. Until now, it remains challenging to obtain Mg-calcite mesocrystals without organic additives and the formation mechanism of Mg-calcite mesocrystals in the ocean is not clear yet. We report here the synthesis of corn-like Mg-calcite mesocrystals from pure amorphous calcium carbonate (ACC) via a facile method only by using Ca2+ and Mg2+. The obtained Mg-calcite is composed of many nanocubes with common crystallographic orientation, which shows very good single crystal feature. In the crystallizing procedure, the ACC nanospheres rapidly agglomerate into Mg-calcite corn-like mesocrystal by oriented attachment (OA) in a certain direction, which belongs to the non-classical nucleation. By this method, the molar ratio of Ca2+ and Mg2+ plays a vital role in the whole crystallization procedure, which may shed a new light on disclosing the mechanism behind for the effect of seawater in the formation of biological Mg-calcite in nature.

Petroleum-based plastics are useful but they pose a great threat to the environment and human health. It is highly desirable yet challenging to develop sustainable structural materials with excellent mechanical and thermal properties for plastic replacement. Here, inspired by nacre’s multiscale architecture, we report a simple and efficient so called “directional deforming assembly” method to manufacture high-performance structural materials with a unique combination of high strength (281 MPa), high toughness (11.5 MPa m1/2), high stiffness (20 GPa), low coefficient of thermal expansion (7 × 10−6 K−1) and good thermal stability. Based on all-natural raw materials (cellulose nanofiber and mica microplatelet), the bioinspired structural material possesses better mechanical and thermal properties than petroleum-based plastics, making it a high-performance and eco-friendly alternative structural material to substitute plastics., It is desirable yet challenging to develop sustainable structural materials to replace petroleum-based plastics. Here, the authors report a facile assembly method for manufacturing high-performance structural materials with a unique combination of high strength, toughness and stiffness.

Although solar-driven water splitting on semiconductor photocatalysts is an attractive route for hydrogen generation, there is a lack of excellent photocatalysts with high visible light activity. Due to their tunable bandgaps suitable for superior visible-light absorption, copper-based quaternary sulfides have been the important candidates. Here, we first assessed the preferred facet of wurtzite Cu-Zn-In-S for photocatalytic hydrogen evolution reaction using the relevant Gibbs free energies determined by first principle calculation. We then developed a colloidal method to synthesize single crystalline wurtzite Cu-Zn-In-S nanobelts (NBs) exposing (0001) facet with the lowest reaction Gibbs energy, as well as Cu-Zn-Ga-S NBs exposing (0001) facet. The obtained single crystalline Cu-Zn-In-S and Cu-Zn-Ga-S NBs exhibit superior hydrogen production activities under visible-light irradiation, which is composition-dependent. Our protocol represents an alternative surface engineering approach to realize efficient solar-to-chemical conversion of single crystalline copper-based multinary chalcogenides., Quaternary sulfides are important candidates for solar-to-H2 conversion due to tunable bandgaps for controllable light absorption. Here, authors prepare single crystalline wurtzite Cu-Zn-In-S and Cu-Zn-Ga-S nanobelts with (0001) facets that show strong photocatalytic H2 production performances.

Summary Plastics play a critical role in daily life but possess a considerably increasing negative impact on the environment and human health. Fabrication of biodegradable and eco-friendly alternatives with competitive properties for plastic substitute is urgently needed. Here, inspired by the hierarchical structure of nacre, we firstly developed a high-performance nacre-inspired composite with high transmittance (83.4% at 550 nm) and high haze (88.8% at 550 nm) via an aerosol-assisted biosynthesis process combined with the hot-press technique. The nacre-inspired composite film combines higher strength (482 MPa) and toughness (17.71 MJ m−3) than most other nacre-inspired films, and can be folded into various shapes without visible failure after unfolding. Moreover, compared with most commercial plastic films, it exhibits a lower thermal expansion coefficient (∼3 ppm K−1) and higher maximum service temperature besides better mechanical properties, which makes it a promising alternative to plastics in many technical fields.

The ever-growing push for sustainable energy has intensified research on catalytic science. Significant developments have been achieved in state-of-the-art catalyst design from the perspective of catalyst materials. Further promotion can be enabled when rethinking and redesigning the catalyst structure with long-range ordering rather than limited to the catalyst material design. Recently, ordered assembled nanostructures have shown advantages over their disordered counterparts in active site exposure and mass transfer. In this opinion article, we revisit and relate orderly assembly to entropy reduction. Recent advances in the engineering of ordered nanostructure assemblies and their applications in electrocatalysis are highlighted, along with discussions of the mechanism of ordering effects. Finally, future research opportunities are provided to encourage further developments in the construction and application of ordered nanostructure assemblies.

ConspectusProgramming nanoscale functional objects into complex, sophisticated heterostructures that tremendously outperform their solo objects and even bring about exotic chemical/physical propert...

Single-atom catalysts (SACs) are of great interest because of their ultrahigh activity and selectivity. However, it is difficult to construct model SACs according to a general synthetic method, and therefore, discerning differences in activity of diverse single-atom catalysts is not straightforward. Herein, a general strategy for synthesis of single-atom metals implanted in N-doped carbon (M1 -N-C; M=Fe, Co, Ni and Cu) has been developed starting from multivariate metal-organic frameworks (MOFs). The M1 -N-C catalysts, featuring identical chemical environments and supports, provided an ideal platform for differentiating the activity of single-atom metal species. When employed in electrocatalytic CO2 reduction, Ni1 -N-C exhibited a very high CO Faradaic efficiency (FE) up to 96.8 % that far surpassed Fe1 -, Co1 - and Cu1 -N-C. Remarkably, the best-performer, Ni1 -N-C, even demonstrated excellent CO FE at low CO2 pressures, thereby representing a promising opportunity for the direct use of dilute CO2 feedstock.

Although nickel-based catalysts display good catalytic capability and excellent corrosion resistance under alkaline electrolytes for water splitting, it is still imperative to enhance their activity for real device applications. Herein, we decorated Ni0.85Se hollow nanospheres onto reduced graphene oxide (RGO) through a hydrothermal route, then annealed this composite at different temperatures (400 °C, NiSe2-400 and 450 °C, NiSe2-450) under argon atmosphere, yielding a kind of NiSe2/RGO composite catalysts. Positron annihilation spectra revealed two types of vacancies formed in this composite catalyst. We found that the NiSe2-400 catalyst with dual Ni-Se vacancies is able to catalyze the oxygen evolution reaction (OER) efficiently, needing a mere 241 mV overpotential at 10 mA·cm−2. In addition, this catalyst exhibits outstanding stability. Computational studies show favorable energy barrier on NiSe2-400, enabling moderate OH− adsorption and O2 desorption, which leads to the enhanced energetics for OER.

Printable elastic conductors promote the wide application of consumable electronic textiles (e-textiles) for pervasive healthcare monitoring and wearable computation. To assure a clean appearance, the e-textiles require a washing process to clean up the dirt after daily use. Thus, it is crucial to develop low-cost printable elastic conductors with strong adhesion to the textiles. Here, we report a composite elastic conductor based on Ag nanowires (NWs) and polyurethane elastomer. The composite could be dispersed into ink and easily printed onto textiles. One-step print could form robust conductive coatings without sealing on the textiles. Interestingly, the regional concentration of Ag NWs within the polyurethane matrix was observed during phase inversion, endowing the elastic conductor with a low percolation threshold of 0.12 vol.% and high conductivity of 3,668 S·cm−1. Thanks to the high adhesion of the elastic conductors, the resulted e-textiles could withstand repeated stretching, folding, and machine washing (20 times) without obvious performance decay, which reveals its potential application in consumable e-textiles.

The increasing demand for the state-of-the-art transparent conductive electrodes has received great interest in synthesizing silver nanowires (AgNWs) with a uniform diameter that exhibit excellent conductance, transparency, flexibility and mechanical ductility. Herein, we report the controllable synthesis of ultrathin AgNWs with high aspect ratio via a polyol-assisted process. The diameter of AgNWs can be continuously modulated from 20 to 80 nm by simply adjusting the aging time. The self-assembled films fabricated by using AgNWs with a diameter of 20 nm as building blocks enable an excellent performance and show a sheet resistance of ∼30 Ω/sq and an optical transmittance of 94%. In addition, such nanowire-based conductive films can keep the excellent flexibility and resistance after bending 10,000 cycles. Similarly, the intelligent dimming films prepared by this AgNW films also have excellent flexibility and stability.

Selective semihydrogenation of alkynes has been a long-term and significant target, yet it remains a great challenge. Herein, bimetallic nanoparticles in a metal–organic framework (MOF), i.e., CuPd...

Single-atom catalysts (SACs) have sparked broad interest recently while the low metal loading poses a big challenge for further applications. Herein, a dual protection strategy has been developed to give high-content SACs by nanocasting SiO2 into porphyrinic metal–organic frameworks (MOFs). The pyrolysis of SiO2@MOF composite affords single-atom Fe implanted N-doped porous carbon (FeSA–N–C) with high Fe loading (3.46 wt%). The spatial isolation of Fe atoms centered in porphyrin linkers of MOF sets the first protective barrier to inhibit the Fe agglomeration during pyrolysis. The SiO2 in MOF provides additional protection by creating thermally stable FeN4/SiO2 interfaces. Thanks to the high-density FeSA sites, FeSA–N–C demonstrates excellent oxygen reduction performance in both alkaline and acidic medias. Meanwhile, FeSA–N–C also exhibits encouraging performance in proton exchange membrane fuel cell, demonstrating great potential for practical application. More far-reaching, this work grants a general synthetic methodology toward high-content SACs (such as FeSA, CoSA, NiSA).

The high surface energy of nanomaterials endows them a metastable nature, which greatly limits their application. However, in some cases, the degradation process derived from the poor stability of nanomaterials offers an unconventional approach to design and obtain functional nanomaterials. Herein, based on the poor stability of ZnSe-[DETA]0.5 hybrid nanobelts, we developed a new strategy to chemically graphitize and functionalize graphene oxide (GO). When ZnSe[DETA]0.5 hybrid nanobelts encountered a strong acid, they were attacked by H+ cations and could release highly reactive Se2− anions into the reaction solution. Like other common reductants (such as N2H4·H2O), these Se2− anions exhibited an excellent ability to restore the structure of GO. The structural restoration of GO was greatly affected by the reaction time, the volume of HCl, and the mass ratio between GO and ZnSe[DETA]0.5 nanobelts. By carefully controlling the reaction process and the post-processing process, we finally obtained several Se-based reduced GO (RGO) nanocomposites (such as ZnSe/Se-RGO, ZnSe-RGO, and Se-RGO) and various selenide/metal-RGO nanocomposites (such as Ag2Se-RGO, Cu2Se-RGO, and Pt-RGO). Although the original structure and composition of ZnSe[DETA]0.5 nanobelts are destroyed, the procedure presents an unconventional way to chemically graphitize and functionalize GO and thus provides a new material synthesis platform for nanocomposites.

Summary Batch hydrothermal reactor is known as a closed system, and what happens in this “black box” is mysterious. Now, by using the tendency of graphene oxide (GO) to align along the flow and the fixation effect of thermoset resin, the hydrothermal annular convection can be inferred from the axisymmetric poloidal structure and GO-assembled annular distribution. Temperature difference and geometric symmetricity of the reactor account for the annular convection, which is also found to be affected by solution viscosity and reactor parameters. Numerical simulations reproduce the annular convection and are used to investigate the parameter space beyond experiments. Plume flows occur at the bottom of the reactor due to flow instability. Irregular and intensive flow is against the synthesis of high-aspect-ratio nanomaterials and monolithic gels. It is noteworthy that large-scale batch hydrothermal synthesis may not be feasible for some nanowires, nanosheets, and particularly gels due to the non-negligible flow influence.

Solar steam generation is an emerging research field to approach the challenge of water shortages all around the world. Abundant light absorber materials have been developed to improve the broadban...

Photoelectrochemical (PEC) hydrogen production is of great interest as an ideal avenue towards clean and renewable energy. However, the instability and low energy conversion efficiency of photoanodes hinder their practical applications. Here we address these issues by introducing a hole extraction layer (HEL) which could rapidly transfer and consume photogenerated holes. The HEL is constructed by reduced graphene oxide (RGO) and other cocatalysts that enable rapid transfer and subsequent consumption of holes, respectively. Specifically, we showcase a high-stability photoanode composed of CdSeTe nanowires (CST NWs) and RGO/PdS nanoparticles (PdS NPs) based HEL. The photoanode achieves excellent photocorrosion resistance, which allows stable hydrogen evolution for > 2 h at 0.5 VRHE.

Three-dimensional (3D) graphene networks are performance boosters for functional nanostructures in energy-related fields. Although tremendous intriguing nanostructures-decorated 3D graphene network...

The general synthesis and control of the coordination environment of single-atom catalysts (SACs) remains a great challenge. Herein, a general host-guest cooperative protection strategy has been developed to construct SACs by introducing polypyrrole (PPy) into a bimetallic metal-organic framework. As an example, the introduction of Mg2+ in MgNi-MOF-74 extends the distance between adjacent Ni atoms; the PPy guests serve as N source to stabilize the isolated Ni atoms during pyrolysis. As a result, a series of single-atom Ni catalysts (named NiSA -Nx -C) with different N coordination numbers have been fabricated by controlling the pyrolysis temperature. Significantly, the NiSA -N2 -C catalyst, with the lowest N coordination number, achieves high CO Faradaic efficiency (98 %) and turnover frequency (1622 h-1 ), far superior to those of NiSA -N3 -C and NiSA -N4 -C, in electrocatalytic CO2 reduction. Theoretical calculations reveal that the low N coordination number of single-atom Ni sites in NiSA -N2 -C is favorable to the formation of COOH* intermediate and thus accounts for its superior activity.

A considerable challenge in the conversion of carbon dioxide into useful fuels comes from the activation of CO2 to CO2 .- or other intermediates, which often requires precious-metal catalysts, high overpotentials, and/or electrolyte additives (e.g., ionic liquids). We report a microwave heating strategy for synthesizing a transition-metal chalcogenide nanostructure that efficiently catalyzes CO2 electroreduction to carbon monoxide (CO). We found that the cadmium sulfide (CdS) nanoneedle arrays exhibit an unprecedented current density of 212 mA cm-2 with 95.5±4.0 % CO Faraday efficiency at -1.2 V versus a reversible hydrogen electrode (RHE; without iR correction). Experimental and computational studies show that the high-curvature CdS nanostructured catalyst has a pronounced proximity effect which gives rise to large electric field enhancement, which can concentrate alkali-metal cations resulting in the enhanced CO2 electroreduction efficiency.

Efficient initiation and resolution of inflammation are crucial for wound repair. However, with using tissue adhesives for wound repair, patients occasionally suffered from delayed healing process because slow elimination of those exogenous adhesives generally leads to chronic inflammation. As the demand for minimal invasive therapy continues to rise, desire for adhesive materials that can effectively reconnect surgical gaps and promote wound regeneration becomes increasingly urgent. Herein, by exploiting the inherent porous structure and performance of adhesion to tissue of mesoporous silica nanoparticles (MSNs), we demonstrate a tissue adhesive that can elicit acute inflammatory response and get eliminated after tissue reformation. With formation of nanocomposites in wound gaps, the injured tissues can get reconnected conveniently. The resultant accelerated healing process verify that the strategy of exploiting unique properties of nanomaterials can effectively promote inflammation resolution and wound repair. This design strategy will inspire more innovative tissue adhesives for clinical applications.

As a non-invasive therapeutic method without penetration-depth limitation, magnetic hyperthermia therapy (MHT) under alternating magnetic field (AMF) is a clinically promising thermal therapy. However, the poor heating conversion efficiency and lack of stimulus–response obstruct the clinical application of magnetofluid-mediated MHT. Here, we develop a ferrimagnetic polyethylene glycol-poly(2-hexoxy-2-oxo-1,3,2-dioxaphospholane) (mPEG-b-PHEP) copolymer micelle loaded with hydrophobic iron oxide nanocubes and emodin (denoted as EMM). Besides an enhanced magnetic resonance (MR) contrast ability (r2 = 271 mM−1 s−1) due to the high magnetization, the specific absorption rate (2518 W/g at 35 kA/m) and intrinsic loss power (6.5 nHm2/kg) of EMM are dozens of times higher than the clinically available iron oxide nanoagents (Feridex and Resovist), indicating the high heating conversion efficiency. Furthermore, this composite micelle with a flowable core exhibits a rapid response to magnetic hyperthermia, leading to an AMF-activated supersensitive drug release. With the high magnetic response, thermal sensitivity and magnetic targeting, this supersensitive ferrimagnetic nanocomposite realizes an above 70% tumor cell killing effect at an extremely low dosage (10 μg Fe/mL), and the tumors on mice are completely eliminated after the combined MHT–chemotherapy.

Electrochemical reduction of carbon dioxide (CO2) to value-added chemicals and fuels offers a potential platform to store renewable energy in chemical bonds and thus a route to carbon recycling. Due to its high efficiency and reasonable economic feasibility, the conversion of CO2 to carbon monoxide (CO) is considered as the most promising candidate reaction in the industrial market. Recently, the understanding of the basic mechanism of CO2 reduction to CO has become clearer, which has also motivated the design principles for better-performing catalysts including morphology, size, grain boundary, and surface engineering. Various catalysts (noble and non-noble metals, transition metal chalcogenides, carbon materials, and molecular catalysts) have been developed to efficiently catalyze the CO2-to-CO conversion. Here we survey recent key progress in CO2-to-CO conversion in the field of electrocatalytic CO2 reduction. We will highlight the principles of designing electrocatalysts for the selective formation of CO, the influence of electrolytes on the selectivity and conversion rate, and the emerging applications of electrolyzers for large-scale CO production. We finally provide an outlook on several development opportunities that could lead to new advancements in this promising research field.

Over the past 150 years, our ability to produce and transform engineered materials has been responsible for our current high standards of living, especially in developed economies. However, we must carefully think of the effects our addiction to creating and using materials at this fast rate will have on the future generations. The way we currently make and use materials detrimentally affects the planet Earth, creating many severe environmental problems. It affects the next generations by putting in danger the future of the economy, energy, and climate. We are at the point where something must drastically change, and it must change now. We must create more sustainable materials alternatives using natural raw materials and inspiration from nature while making sure not to deplete important resources, i.e. in competition with the food chain supply. We must use less materials, eliminate the use of toxic materials and create a circular materials economy where reuse and recycle are priorities. We must develop sustainable methods for materials recycling and encourage design for disassembly. We must look across the whole materials life cycle from raw resources till end of life and apply thorough life cycle assessments (LCAs) based on reliable and relevant data to quantify sustainability. We need to seriously start thinking of where our future materials will come from and how could we track them, given that we are confronted with resource scarcity and geographical constrains. This is particularly important for the development of new and sustainable energy technologies, key to our transition to net zero. Currently ‘critical materials’ are central components of sustainable energy systems because they are the best performing. A few examples include the permanent magnets based on rare earth metals (Dy, Nd, Pr) used in wind turbines, Li and Co in Li-ion batteries, Pt and Ir in fuel cells and electrolysers, Si in solar cells just to mention a few. These materials are classified as ‘critical’ by the European Union and Department of Energy. Except in sustainable energy, materials are also key components in packaging, construction, and textile industry along with many other industrial sectors. This roadmap authored by prominent researchers working across disciplines in the very important field of sustainable materials is intended to highlight the outstanding issues that must be addressed and provide an insight into the pathways towards solving them adopted by the sustainable materials community. In compiling this roadmap, we hope to aid the development of the wider sustainable materials research community, providing a guide for academia, industry, government, and funding agencies in this critically important and rapidly developing research space which is key to future sustainability., The authors would like to thank The Faraday Institution ReLiB Project Grant Numbers FIRG005 and FIRG006, the UKRI Interdisciplinary Circular Economy Centre for Technology Metals (Met4Tech) Grant No. EP/V011855/1 and the EPSRC Critical Elements and Materials Network (CREAM) EP/R020140/1 for providing financial assistance for this research.

Assembling various nanowires together, enabling the assemblies with tailored optical, electrical, and multifunctional properties, represents a promising technology for next generation multifunctional electronics. Here we demonstrate a novel multicolor electrochromic device by coassembling W18O49 and V2O5 nanowires using solution-based Langmuir-Blodgett technique. The transparent W18O49 nanowire film became orange with the increasing addition of V2O5 nanowires and the film underwent a dynamic color change (orange, green, and gray) on application of different electrochemical biases of 2, 0, and -0.5 V (vs Ag/AgCl). Both the transmittance and color of the device can be easily controlled by manipulating the layers of coassembled nanowires and the ratios between the two nanowires. On the basis of this approach, different patterns can be easily fabricated with the addition of corresponding masks, and the solid electrochromic device is assembled, suggesting its significant potentials in smart windows and multicolor electrochromic displays.

Ubiquitous petrochemical-based plastics pose a potential threat to ecosystems. In response, bioderived and degradable polymeric materials are being developed, but their mechanical and thermal properties cannot compete with those of existing petrochemical-based plastics, especially those used as structural materials. Herein, we report a biodegradable plant cellulose nanofiber (CNF)-derived polymeric structural material with high-density reversible interaction networks between nanofibers, exhibiting mechanical and thermal properties better than those of existing petrochemical-based plastics. This all-green material has substantially improved flexural strength (∼300 MPa) and modulus (∼16 GPa) compared with those of existing petrochemical-based plastics. Its average thermal expansion coefficient is only 7 × 10-6 K-1, which is more than 10 times lower than those of petrochemical-based plastics, indicating its dimension is almost unchanged when heated, and thus, it has a thermal dimensional stability that is better than those of plastics. As a fully bioderived and degradable material, the all-green material offers a more sustainable high-performance alternative to petrochemical-based plastics.

Owing to their outstanding comprehensive performance, polyimide (PI) composite films are widely used on the external surfaces of spacecraft to protect them from the adverse conditions of low Earth orbit (LEO). However, current PI composite films have inadequate mechanical properties and atomic oxygen (AO) resistance. Herein, this work fabricates a new PI-based nanocomposite film with greatly enhanced mechanical properties and AO resistance by integrating mica nanosheets with PI into a unique double-layer nacre-inspired structure with a much higher density of mica nanosheets in the top layer. In addition, the unique microstructure and the intrinsic properties of mica also impart the nanocomposite film with favorable ultraviolet and high-temperature resistance. The comprehensive performance of this material is superior to those of pure PI, single-layer PI-mica, and previously reported PI-based composite films. Thus, the double-layer nanocomposite film displays great potential as an aerospace material for use in LEO.

Photoelectrochemical catalysis is an attractive way to provide direct hydrogen production from solar energy. However, solar conversion efficiencies are hindered by the fact that light harvesting has so far been of limited efficiency in the near-infrared region as compared to that in the visible and ultraviolet regions. Here we introduce near-infrared-active photoanodes that feature lattice-matched morphological hetero-nanostructures, a strategy that improves energy conversion efficiency by increasing light-harvesting spectral range and charge separation efficiency simultaneously. Specifically, we demonstrate a near-infrared-active morphological heterojunction comprised of BiSeTe ternary alloy nanotubes and ultrathin nanosheets. The heterojunction’s hierarchical nanostructure separates charges at the lattice-matched interface of the two morphological components, preventing further carrier recombination. As a result, the photoanodes achieve an incident photon-to-current conversion efficiency of 36% at 800 nm in an electrolyte solution containing hole scavengers without a co-catalyst., The solar conversion efficiencies of photoelectrochemical catalysis are hindered by the light harvesting range. Here, the authors use near-infrared-active photoanodes that feature lattice-matched morphological hetero-nanostructures to realize efficient photoelectrochemical hydrogen production.

Amorphous calcium carbonate (ACC) plays a key role as transient precursor in the early stages of biogenic calcium carbonate formation in nature. However, due to its instability in aqueous solution, there is still rare success to utilize ACC in biomedicine. Here, we report the mutual effect between paramagnetic gadolinium ions and ACC, resulting in ultrafine paramagnetic amorphous carbonate nanoclusters (ACNC) in the presence of both gadolinium occluded highly hydrated ACC-like environment and poly(acrylic acid). Gadolinium is confirmed to enhance the water content in ACC, and the high water content of ACNC (23 molecules H2O per 1 Gd) contributes to the much enhanced magnetic resonance imaging (MRI) contrast efficiency compared with commercially available gadolinium-based contrast agents. Furthermore, the enhanced T1 weighted MRI performance and biocompatibility of ACNC are further evaluated in various animals including rat, rabbit and beagle dog, in combination with promising safety in vivo. Overall, exceptionally facile mass-productive ACNC exhibits superb imaging performance and impressive stability, which provides a promising strategy to design MR contrast agents.

Dynamic soft materials are requisite components not only for the survival of organisms in complicated natural environments but also for the advancement and operation of smart devices. A recently published article ( Zhao et al. ) reports new tunable polymeric materials exhibiting excellent reversible properties when the network hydration state is varied.

Many platinum group metal-free inorganic catalysts have demonstrated high intrinsic activity for diverse important electrode reactions, but their practical use often suffers from undesirable structural degradation and hence poor stability, especially in acidic media. We report here an alkali-heating synthesis to achieve phase-mixed cobalt diselenide material with nearly homogeneous distribution of cubic and orthorhombic phases. Using water electroreduction as a model reaction, we observe that the phase-mixed cobalt diselenide reaches the current density of 10 milliamperes per square centimeter at overpotential of mere 124 millivolts in acidic electrolyte. The catalyst shows no sign of deactivation after more than 400 h of continuous operation and the polarization curve is well retained after 50,000 potential cycles. Experimental and computational investigations uncover a boosted covalency between Co and Se atoms resulting from the phase mixture, which substantially enhances the lattice robustness and thereby the material stability. The findings provide promising design strategy for long-lived catalysts in acid through crystal phase engineering., Noble-metal-free catalysts often show stability issues in acidic media due to structural degradation. Here authors show that phase-mixed engineering of cobalt diselenide electrocatalysts can enable greater covalency of Co-Se bonds and improve robustness for catalyzing hydrogen evolution in acid.

Over the past decades, nanomaterials have been proven to have superior properties, because of their unique structural features differentiating from atoms and bulk materials, and their large-scale p...

The anode oxygen evolution reaction (OER) is known to largely limit the efficiency of electrolyzers owing to its sluggish kinetics. While crystalline metal oxides are promising as OER catalysts, their amorphous phases also show high activities. Efforts to produce amorphous metal oxides have progressed slowly, and how an amorphous structure benefits the catalytic performances remains elusive. Now the first scalable synthesis of amorphous NiFeMo oxide (up to 515 g in one batch) is presented with homogeneous elemental distribution via a facile supersaturated co-precipitation method. In contrast to its crystalline counterpart, amorphous NiFeMo oxide undergoes a faster surface self-reconstruction process during OER, forming a metal oxy(hydroxide) active layer with rich oxygen vacancies, leading to superior OER activity (280 mV overpotential at 10 mA cm-2 in 0.1 m KOH). This opens up the potential of fast, facile, and scale-up production of amorphous metal oxides for high-performance OER catalysts.

Summary Guided bone regeneration (GBR) membranes have been commonly used for bone defect repair in clinical medicine. However, the existing GBR membranes are often limited by weak mechanical strength, poor antibacterial effect, overquick degradation or non-degradation, etc. Here, inspired by natural nacre and the most commonly used GBR membrane (Bio-Gide), we report a new kind of GBR membrane fabricated by combining evaporation-induced self-assembly with a subsequent ice-templating procedure. Similar to the Bio-Gide membrane, it also consists of a bilayer structure including a compact nacre-like layer and a porous layer. Furthermore, it exhibits high mechanical properties and other functions not achieved by the Bio-Gide membrane. The obtained high mechanical properties and multiple functions, including effective bacteriostasis, appropriate degradation rate, and biocompatibility, are superior to those of previously reported GBR membranes. This multifunctional bilayer membrane, fabricated via a simple and straightforward method, may be an appropriate candidate as a bioactive GBR membrane for clinical application.

Summary Biomimetic bulk structural materials have been paid increasing attention for their huge application prospects. Integrating close-to-ideal, ultrathin, and flexible nanostructured units into high-performance nacreous bulk nanocomposites is worth considering yet remains challenging due to the elusive micro- and nano-interface connections. Here, by introducing a multiscale soft-rigid polymer dual-network interfacial design strategy that enables us to appropriately reinforce the nanoscale building blocks or their bridging, we can construct a type of nacreous bulk nanocomposites with tunable mechanical properties in the mild, eco-friendly, and highly efficient bottom-up assembly process. The resultant nanocomposites can achieve continuously reinforced mechanical transformation without experiencing environmentally threatening interfacial manipulation processes. This interfacial design strategy, supported by sufficient experiments and simulations, endows the assembled nacreous nanocomposite with superior mechanical enhancement and improved stability under high humidity and temperature conditions. Combined with the scalable assembly technique, it will pave the way for the design of high-performance biomimetic bulk nanocomposites for structural applications.

Molybdenum disulfide (MoS2) has been intensively investigated for its high theoretical capacity as an advanced anode material for lithium storage. However, the low electronic conductivity and frail layered structure give rise to its poor cycling stability and low rate performance. Herein, by taking advantages of the porous structure and the high N content of metal-organic frameworks (MOFs) derivatives, a facile and scalable method combining electrospinning and following a hydrothermal process was developed to fabricate MoS2-based composite fibers, in which ultrathin MoS2 nanoplates were vertically assembled on the polyacrylonitrile-MOF-derived N-doped porous carbon nanofibers (PCNF). As expected, benefiting from the hierarchical structure of PCNF and the synergies between MoS2 and PCNF, the obtained PCNF@MoS2 exhibited high capacity and cycling performance in a lithium battery.

Summary Inspired by microstructures of polar bear hair, herein, we describe a simple solution-based strategy to fabricate a macroscopic-scale and lightweight carbon tube aerogel with super-elasticity and excellent thermal insulation. The microstructure-derived thermal conductivity and super-elasticity are strongly dependent on the shell thickness of the interconnected tubes, as well as the aperture of the aerogel. Remarkably, the optimized aerogel can maintain structural integrity after more than one million compress-release cycles at 30% strain and 10,000 cycles at 90% strain. Moreover, this biomimetic aerogel offers a fast and accurate dynamic piezoresistive response to broad bandwidth frequency forces. Particularly, the super-elasticity is further confirmed by its fastest rebounding speed of 1,434 mm s −1 among the traditional elastic materials measured by a standard falling steel ball. Furthermore, the optimized minimum thermal conductivity is as low as 23 mW m −1 K −1 which performs better than the thermal conductivity of dry air.