Examining the Impact of 3D Multi-Arm Small Molecules on PM6 : Y6 Blend Reveals the Key Requirements for Their Electronic Properties.

While the emergence of PM6 : Y6 active layer re-energized the organic photovoltaic community, excessive aggregation of Y6 molecules induced by their strong intermolecular interactions has limited the performance of PM6 : Y6-based organic solar cells (OSCs). Adding 3D multi-arm small-molecule acceptors is an effective strategy to inhibit such aggregation. However, to maximize OSC efficiency, these molecules should also contribute to the electronic processes.

Upcycling Polyethylene to High-Purity Hydrogen under Ambient Conditions via Mechanocatalysis.

Polyethylene (PE) is the most abundant plastic waste, and its conversion to hydrogen (H) offers a promising route for clean energy generation. However, PE decomposition typically requires high temperatures due to its strong chemical bonds, leading to significant carbon emissions and low H selectivity (theoretically less than 75 vol % after accounting for further steam-reforming reactions). Here, we report a mechanocatalytic strategy that upcycles PE into high-purity H (99.

Achieving a Thermodynamic Self-Regulation Dynamic Adsorption Mechanism for Ammonia Synthesis through Selective Orbital Coupling.

With the continuous pursuing on the improvement of catalytic activity, a catalyst performed exceeding catalytic volcano plots is desired, while it is impeded by the adsorption-energy scaling relations of reaction intermediates. Numerous efforts have been focused on optimizing the initial and final intermediates to circumvent the scaling relations for an improved performance. For a step forward, simultaneously optimizing all intermediates is essential to explore the theoretical maximum of catalytic activity.

Dual-Intermetallic Heterostructure on Hierarchical Nanoporous Metal for Highly Efficient Alkaline Hydrogen Electrocatalysis.

Constructing well-defined active multisites is an effective strategy to break linear scaling relationships to develop high-efficiency catalysts toward multiple-intermediate reactions. Here, dual-intermetallic heterostructure composed of tungsten-bridged CoW and WNi intermetallic compounds seamlessly integrated on hierarchical nanoporous nickel skeleton is reported as a high-performance nonprecious electrocatalyst for alkaline hydrogen evolution and oxidation reactions. By virtue of interfacial tungsten atoms configuring contiguous multisites with proper adsorptions of hydrogen and hydroxyl intermediates to accelerate water dissociation/combination and column-nanostructured nickel skeleton facilitating electron and ion/molecule transportations, nanoporous nickel-supported CoW-WNi heterostructure exhibits exceptional hydrogen electrocatalysis in alkaline media, with outstanding durability and impressive catalytic activities for hydrogen oxidation reaction (geometric exchange current density of ≈6.

Lamellar Nanoporous Metal/Intermetallic Compound Heterostructure Regulating Dendrite-Free Zinc Electrodeposition for Wide-Temperature Aqueous Zinc-Ion Battery.

Aqueous zinc-ion batteries are attractive post-lithium battery technologies for grid-scale energy storage because of their inherent safety, low cost and high theoretical capacity. However, their practical implementation in wide-temperature surroundings persistently confronts irregular zinc electrodeposits and parasitic side reactions on metal anode, which leads to poor rechargeability, low Coulombic efficiency and short lifespan. Here, this work reports lamellar nanoporous Cu/AlCu heterostructure electrode as a promising anode host material to regulate high-efficiency and dendrite-free zinc electrodeposition and stripping for wide-temperatures aqueous zinc-ion batteries.

In Situ Engineering Multifunctional Active Sites of Ruthenium-Nickel Alloys for pH-Universal Ampere-Level Current-Density Hydrogen Evolution.

Developing robust non-platinum electrocatalysts with multifunctional active sites for pH-universal hydrogen evolution reaction (HER) is crucial for scalable hydrogen production through electrochemical water splitting. Here ultra-small ruthenium-nickel alloy nanoparticles steadily anchored on reduced graphene oxide papers (Ru-Ni/rGOPs) as versatile electrocatalytic materials for acidic and alkaline HER are reported. These Ru-Ni alloy nanoparticles serve as pH self-adaptive electroactive species by making use of in situ surface reconstruction, where surface Ni atoms are hydroxylated to produce bifunctional active sites of Ru-Ni(OH) for alkaline HER, and selectively etched to form monometallic Ru active sites for acidic HER, respectively.

Dynamic Molecular Interphases Regulated by Trace Dual Electrolyte Additives for Ultralong-Lifespan and Dendrite-Free Zinc Metal Anode.

Metallic zinc is a promising anode material for rechargeable aqueous multivalent metal-ion batteries due to its high capacity and low cost. However, the practical use is always beset by severe dendrite growth and parasitic side reactions occurring at anode/electrolyte interface. Here we demonstrate dynamic molecular interphases caused by trace dual electrolyte additives of D-mannose and sodium lignosulfonate for ultralong-lifespan and dendrite-free zinc anode.

Benzoquinone-Lubricated Intercalation in Manganese Oxide for High-Capacity and High-Rate Aqueous Aluminum-Ion Battery.

Aqueous aluminum-ion batteries are attractive post-lithium battery technologies for large-scale energy storage in virtue of abundant and low-cost Al metal anode offering ultrahigh capacity via a three-electron redox reaction. However, state-of-the-art cathode materials are of low practical capacity, poor rate capability, and inadequate cycle life, substantially impeding their practical use. Here layered manganese oxide that is pre-intercalated with benzoquinone-coordinated aluminum ions (BQ-AlMnO) as a high-performance cathode material of rechargeable aqueous aluminum-ion batteries is reported.

Ultrafast Nucleation Reverses Dissolution of Transition Metal Ions for Robust Aqueous Batteries.

The dissolution of transition metal ions causes the notorious peeling of active substances and attenuates electrochemical capacity. Frustrated by the ceaseless task of pushing a boulder up a mountain, Sisyphus of the Greek myth yearned for a treasure to be unearthed that could bolster his efforts. Inspirationally, by using ferricyanide ions (Fe(CN)) in an electrolyte as a driving force and taking advantage of the fast nucleation rate of copper hexacyanoferrate (CuHCF), we successfully reversed the dissolution of Fe and Cu ions that typically occurs during cycling.

Achieving volatile potassium promoted ammonia synthesis via mechanochemistry.

Potassium oxide (KO) is used as a promotor in industrial ammonia synthesis, although metallic potassium (K) is better in theory. The reason KO is used is because metallic K, which volatilizes around 400 °C, separates from the catalyst in the harsh ammonia synthesis conditions of the Haber-Bosch process. To maximize the efficiency of ammonia synthesis, using metallic K with low temperature reaction below 400 °C is prerequisite.

Lamella-heterostructured nanoporous bimetallic iron-cobalt alloy/oxyhydroxide and cerium oxynitride electrodes as stable catalysts for oxygen evolution.

Developing robust nonprecious-metal electrocatalysts with high activity towards sluggish oxygen-evolution reaction is paramount for large-scale hydrogen production via electrochemical water splitting. Here we report that self-supported laminate composite electrodes composed of alternating nanoporous bimetallic iron-cobalt alloy/oxyhydroxide and cerium oxynitride (FeCo/CeON) heterolamellas hold great promise as highly efficient electrocatalysts for alkaline oxygen-evolution reaction. By virtue of three-dimensional nanoporous architecture to offer abundant and accessible electroactive CoFeOOH/CeON heterostructure interfaces through facilitating electron transfer and mass transport, nanoporous FeCo/CeON composite electrodes exhibit superior oxygen-evolution electrocatalysis in 1 M KOH, with ultralow Tafel slope of ~33 mV dec.

Interface Reversible Electric Field Regulated by Amphoteric Charged Protein-Based Coating Toward High-Rate and Robust Zn Anode.

Metallic interface engineering is a promising strategy to stabilize Zn anode via promoting Zn uniform deposition. However, strong interactions between the coating and Zn and sluggish transport of Zn lead to high anodic polarization. Here, we present a bio-inspired silk fibroin (SF) coating with amphoteric charges to construct an interface reversible electric field, which manipulates the transfer kinetics of Zn and reduces anodic polarization.

Surface-Alloyed Nanoporous Zinc as Reversible and Stable Anodes for High-Performance Aqueous Zinc-Ion Battery.

Metallic zinc (Zn) is one of the most attractive multivalent-metal anode materials in post-lithium batteries because of its high abundance, low cost and high theoretical capacity. However, it usually suffers from large voltage polarization, low Coulombic efficiency and high propensity for dendritic failure during Zn stripping/plating, hindering the practical application in aqueous rechargeable zinc-metal batteries (AR-ZMBs). Here we demonstrate that anionic surfactant-assisted in situ surface alloying of Cu and Zn remarkably improves Zn reversibility of 3D nanoporous Zn electrodes for potential use as high-performance AR-ZMB anode materials.

Aluminum-copper alloy anode materials for high-energy aqueous aluminum batteries.

Aqueous aluminum batteries are promising post-lithium battery technologies for large-scale energy storage applications because of the raw materials abundance, low costs, safety and high theoretical capacity. However, their development is hindered by the unsatisfactory electrochemical behaviour of the Al metal electrode due to the presence of an oxide layer and hydrogen side reaction. To circumvent these issues, we report aluminum-copper alloy lamellar heterostructures as anode active materials.

Synergistic Effect of Active Sites of Double-Atom Catalysts for Nitrogen Reduction Reaction.

Nitrogen fixation to produce ammonia is a vital process since nitrogen is an essential element for the human body. Industrial nitrogen fixation mainly relies on the Haber-Bosch process. However, this process requires huge energy consumption and leads to pollution emission.

Steric Hindrance- and Work Function-Promoted High Performance for Electrochemical CO Methanation on Antisite Defects of MoS and WS.

CO methanation from electrochemical CO reduction reaction (CORR) is significant for sustainable environment and energy, but electrocatalysts with excellent selectivity and activity are still lacking. Selectivity is sensitive to the structure of active sites, and activity can be tailored by work function. Moreover, intrinsic active sites usually possess relatively high concentration compared to artificial ones.

Spontaneously separated intermetallic CoMo from nanoporous copper as versatile electrocatalysts for highly efficient water splitting.

Developing robust nonprecious electrocatalysts towards hydrogen/oxygen evolution reactions is crucial for widespread use of electrochemical water splitting in hydrogen production. Here, we report that intermetallic CoMo spontaneously separated from hierarchical nanoporous copper skeleton shows genuine potential as highly efficient electrocatalysts for alkaline hydrogen/oxygen evolution reactions in virtue of in-situ hydroxylation and electro-oxidation, respectively. The hydroxylated intermetallic CoMo has an optimal hydrogen-binding energy to facilitate adsorption/desorption of hydrogen intermediates for hydrogen molecules.

Lamella-nanostructured eutectic zinc-aluminum alloys as reversible and dendrite-free anodes for aqueous rechargeable batteries.

Metallic zinc is an attractive anode material for aqueous rechargeable batteries because of its high theoretical capacity and low cost. However, state-of-the-art zinc anodes suffer from low coulombic efficiency and severe dendrite growth during stripping/plating processes, hampering their practical applications. Here we show that eutectic-composition alloying of zinc and aluminum as an effective strategy substantially tackles these irreversibility issues by making use of their lamellar structure, composed of alternating zinc and aluminum nanolamellas.

Intermetallic CuZr Clusters Anchored on Hierarchical Nanoporous Copper as Efficient Catalysts for Hydrogen Evolution Reaction.

Designing highly active and robust platinum-free electrocatalysts for hydrogen evolution reaction is vital for large-scale and efficient production of hydrogen through electrochemical water splitting. Here, we report nonprecious intermetallic CuZr clusters that are in situ anchored on hierarchical nanoporous copper (NP Cu/CuZr) for efficient hydrogen evolution in alkaline medium. By virtue of hydroxygenated zirconium atoms activating their nearby Cu-Cu bridge sites with appropriate hydrogen-binding energy, the CuZr clusters have a high electrocatalytic activity toward the hydrogen evolution reaction.

Flexible Co-Mo-N/Au Electrodes with a Hierarchical Nanoporous Architecture as Highly Efficient Electrocatalysts for Oxygen Evolution Reaction.

Designing highly active and robust electrocatalysts for oxygen evolution reaction (OER) is crucial for many renewable energy storage and conversion devices. Here, self-supported monolithic hybrid electrodes that are composed of bimetallic cobalt-molybdenum nitride nanosheets vertically aligned on 3D and bicontinuous nanoporous gold (NP Au/CoMoN ) are reported as highly efficient electrocatalysts to boost the sluggish reaction kinetics of water oxidation in alkaline media. By virtue of the constituent CoMoN nanosheets having large accessible CoMoO surface with remarkably enhanced electrocatalytic activity and the nanoporous Au skeleton facilitating electron transfer and mass transport, the NP Au/CoMoN electrode exhibits superior OER electrocatalysis in 1 m KOH, with low onset overpotential (166 mV) and Tafel slope (46 mV dec ).

Dual-phase nanostructuring of layered metal oxides for high-performance aqueous rechargeable potassium ion microbatteries.

Aqueous rechargeable microbatteries are promising on-chip micropower sources for a wide variety of miniaturized electronics. However, their development is plagued by state-of-the-art electrode materials due to low capacity and poor rate capability. Here we show that layered potassium vanadium oxides, KVO·nHO, have an amorphous/crystalline dual-phase nanostructure to show genuine potential as high-performance anode materials of aqueous rechargeable potassium-ion microbatteries.

Extraordinary pseudocapacitive energy storage triggered by phase transformation in hierarchical vanadium oxides.

Pseudocapacitance holds great promise for improving energy densities of electrochemical supercapacitors, but state-of-the-art pseudocapacitive materials show capacitances far below their theoretical values and deliver much lower levels of electrical power than carbon-based materials due to poor cation accessibility and/or long-range electron transferability. Here we show that in situ corundum-to-rutile phase transformation in electron-correlated vanadium sesquioxide can yield nonstoichiometric rutile vanadium dioxide layers that are composed of highly sodium ion accessible oxygen-deficiency quasi-hexagonal tunnels sandwiched between conductive rutile slabs. This unique structure serves to boost redox and intercalation kinetics for extraordinary pseudocapacitive energy storage in hierarchical isomeric vanadium oxides, leading to a high specific capacitance of ~1856 F g (almost sixfold that of the pristine vanadium sesquioxide and dioxide) and a bipolar charge/discharge capability at ultrafast rates in aqueous electrolyte.

Scalable Nanoporous (PtNi)Al Intermetallic Compounds as Highly Active and Stable Catalysts for Oxygen Electroreduction.

Author: Bimetallic platinum-nickel (Pt-Ni) alloys as oxygen reduction reaction (ORR) electrocatalysts show genuine potential to boost widespread use of low-temperature fuel cells in vehicles by virtue of their high catalytic activity. However, their practical implementation encounters primary challenges in structural and catalytic durability caused by the low formation heat of Pt-Ni alloys. Here, we report nanoporous (NP) (PtNi)Al intermetallic nanoparticles as oxygen electroreduction catalyst NP (PtNi)Al, which circumvents this problem by making use of the extraordinarily negative formation heats of Pt-Al and Ni-Al bonds.

Ultrahigh-Power Pseudocapacitors Based on Ordered Porous Heterostructures of Electron-Correlated Oxides.

Nanostructured transition-metal oxides can store high-density energy in fast surface redox reactions, but their poor conductivity causes remarkable reductions in the energy storage of most pseudocapacitors at high power delivery (fast charge/discharge rates). Here it is shown that electron-correlated oxide hybrid electrodes made of nanocrystalline vanadium sesquioxide and manganese dioxide with 3D and bicontinuous nanoporous architecture (NP VO/MnO) have enhanced conductivity because of metallization of electron-correlated VO skeleton via insulator-to-metal transition. The conductive VO skeleton at ambient temperature enables fast electron and ion transports in the entire electrode and facilitates charge transfer at abundant VO/MnO interface.