Ecofriendly, Highly Selective Lithium Extraction by Redox-Mediated Electrodialysis.

The rapid proliferation of lithium battery applications has underscored the critical role of lithium supply in the transition to industrial electrification. Existing lithium production methods encounter significant challenges in efficiency, scalability, environmental impact, and cost. The integration of redox-mediated electrodialysis with a dense ceramic LiSrTaHfO perovskite membrane, distinguished by its unique lattice structure allowing only lithium-ion exchange and transport, enables efficient, highly lithium-selective extraction directly from a diversity of resources including seawater and various brines.

Ferrocene Bis(Sulfonate) Salt as Redoxmer for Fast and Steady Redox Flow Desalination.

Desalination is considered a promising solution to alleviate water shortages, yet current methods are often restricted, due to challenges like high energy consumption, significant cost, or limited desalination capacity. In this study, we present a novel approach of redox flow desalination (RFD) utilizing the highly aqueous-soluble and reversible redox-active compound, potassium 1,1'-bis(sulfonate) ferrocene (1,1'-FcDS). This water-soluble organic compound yielded stable and rapid desalination, sustaining extended operation without notable decay and achieving an impressive desalination rate of up to 457.

Non-thermal plasma-assisted rapid hydrogenolysis of polystyrene to high yield ethylene.

The evergrowing plastic production and the caused concerns of plastic waste accumulation have stimulated the need for waste plastic chemical recycling/valorization. Current methods suffer from harsh reaction conditions and long reaction time. Herein we demonstrate a non-thermal plasma-assisted method for rapid hydrogenolysis of polystyrene (PS) at ambient temperature and atmospheric pressure, generating high yield (>40 wt%) of C-C hydrocarbons and ethylene being the dominant gas product (Selectivity of ethylene, S > 70%) within ~10 min.

An Electrochemical Ethylamine/Acetonitrile Redox Method for Ambient Hydrogen Storage.

Hydrogen storage presents a major difficulty in the development of hydrogen economy. Herein, we report a new electrochemical ethylamine/acetonitrile redox method for hydrogen storage with an 8.9 wt % theoretical storage capacity under ambient conditions.

Fingerprinting the Ammonia Synthesis Pathway Using Spatiotemporal Electrostatic Potential Distribution of Intermediates.

It remains a research challenge in determining the catalytic reaction mechanisms primarily caused by the difficulty to experimentally identify active intermediates with current analytic characterizations. Although computational chemistry has provided an alternative approach to simulate the catalysis process and achieve insights into the reaction pathways, the simulation results would not be conclusive without experimental evidence. Herein, we investigate spatiotemporal electrostatic potential (ESP) distribution surrounding reacting molecules during the catalysis process and suggest its use as a fingerprint to help differentiate and identify active intermediates.

Two-Dimensional Metal Organic Framework Nanosheets as Bifunctional Catalyst for Electrochemical and Photoelectrochemical Water Oxidation.

Electrochemical (EC) and photoelectrochemical (PEC) water splitting represent promising strategies for renewable energy conversion and fuel production and require design of efficient catalysts for the oxygen evolution reaction (OER). Herein, we report the synthesis of two-dimensional (2D) Co-based metal organic framework (Co-MOF) nanosheets and their bifunctional catalytic properties for both EC and PEC OER. Benefiting from the large surface area and abundant isolated metal active sites, the Co-MOF nanosheets exhibited excellent OER activity and stability.

Properties of amorphous iron phosphate in pseudocapacitive sodium ion removal for water desalination.

Capacitive deionization (CDI) is an energy saving and environmentally friendly technology for water desalination. However, classical CDI is challenged by a low salt removal capacity. To improve the desalination capacity, electrode materials utilizing the battery mechanism for salt ion removal have emerged as a new direction more recently.

A vacuum impregnation method for synthesizing octahedral PtCuNi nanoparticles on mesoporous carbon support and the oxygen reduction reaction electrocatalytic properties.

Mesoporous carbon (MPC) nanomaterials, with large specific surface area, excellent conductivity and stability, and effective mass transfer are beneficial for use as catalyst support in electrochemical oxygen reduction reaction (ORR) for fuel cell applications. However, MPC utilization was limited by difficulties in loading catalyst nanoparticles within the MPC pores while simultaneously controlling critical particle parameters such as size and distribution. In this study we report a new vacuum impregnation method combined with solid-state chemistry synthesis for preparing highly active ORR catalyst nanoparticles on MPC supports.

Unconventional p-d Hybridization Interaction in PtGa Ultrathin Nanowires Boosts Oxygen Reduction Electrocatalysis.

Alloying 3d transition metals with Pt has been discovered as an effective strategy to boost the catalytic activity in oxygen reduction reaction (ORR), which, however, often raises the insufficient catalyst durability issue due to rapid leaching of the 3d metal elements. To overcome this issue and realize enhancements in both the activity and the durability properties, here we report a new catalytic structure based on PtGa ultrathin alloy nanowires (NWs), which feature an unconventional strong p-d hybridization interaction. Relative to commercial Pt catalyst, the optimum PtGa NWs catalyst exhibited 10.

Dual-Site Cascade Oxygen Reduction Mechanism on SnO /Pt-Cu-Ni for Promoting Reaction Kinetics.

Designing highly active oxygen reduction reaction (ORR) catalysts is crucial to boost the fuel cell economy. Previous research has mainly focused on Pt-based alloy catalysts in which surface Pt is the solely active site and the activity improvement was challenged by the discovered scaling relationship. Herein we report a new concept of utilizing dual active sites for the ORR and demonstrate its effectiveness by synthesizing a SnO /Pt-Cu-Ni heterojunctioned catalyst.

Designing Highly Efficient and Long-Term Durable Electrocatalyst for Oxygen Evolution by Coupling B and P into Amorphous Porous NiFe-Based Material.

Oxygen evolution reaction (OER) is of great significance for hydrogen production via water electrolysis, which, however, demands development of highly active, durable, and cost-effective electrocatalysts in order to stride into a renewable energy era. Herein, highly efficient and long-term durable OER by coupling B and P into an amorphous porous NiFe-based electrocatalyst is reported, which possesses an amorphous porous metallic bulk structure and high corrosion resistance, and overcomes the issues associated with currently used catalyst nanomaterials. The PB codoping in the activated NiFePB (a-NiFePB) delocalizes both Fe and Ni at Fermi energy level and enhances p-d hybridization as simulated by density functional theory calculations.

Deconvolution of octahedral PtNi nanoparticle growth pathway from in situ characterizations.

Understanding the growth pathway of faceted alloy nanoparticles at the atomic level is crucial to morphology control and property tuning. Yet, it remains a challenge due to complexity of the growth process and technical limits of modern characterization tools. We report a combinational use of multiple cutting-edge in situ techniques to study the growth process of octahedral PtNi nanoparticles, which reveal the particle growth and facet formation mechanisms.

High-Performance Transition Metal Phosphide Alloy Catalyst for Oxygen Evolution Reaction.

Oxygen evolution reaction (OER) is a pivotal process in many energy conversion and storage techniques, such as water splitting, regenerative fuel cells, and rechargeable metal-air batteries. The synthesis of stable, efficient, non-noble metal-based electrocatalysts for OER has been a long-standing challenge. In this work, a facile and scalable method to synthesize hollow and conductive iron-cobalt phosphide (Fe-Co-P) alloy nanostructures using an Fe-Co metal organic complex as a precursor is described.

Free-Standing Holey Ni(OH) Nanosheets with Enhanced Activity for Water Oxidation.

Electrochemical water oxidation is the key technology in water-splitting reactions and rechargeable metal-air batteries, which is very attractive for renewable energy conversion and storage. Replacement of precious catalysts with cost-effective and highly active alternatives is still a great challenge. Herein, based on theoretical predictions, holey structures are designed and fabricated on the free-standing conventional 2D OER catalyst.

Achieving Remarkable Activity and Durability toward Oxygen Reduction Reaction Based on Ultrathin Rh-Doped Pt Nanowires.

The research of active and sustainable electrocatalysts toward oxygen reduction reaction (ORR) is of great importance for industrial application of fuel cells. Here, we report a remarkable ORR catalyst with both excellent mass activity and durability based on sub 2 nm thick Rh-doped Pt nanowires, which combine the merits of high utilization efficiency of Pt atoms, anisotropic one-dimensional nanostructure, and doping of Rh atoms. Compared with commercial Pt/C catalyst, the Rh-doped Pt nanowires/C catalyst shows a 7.

More accurate depiction of adsorption energy on transition metals using work function as one additional descriptor.

The reaction mechanism and properties of a catalytic process are primarily determined by the interactions between reacting species and catalysts. However, the interactions are often challenging to be experimentally measured, especially for unstable intermediates. Therefore, it is of significant importance to establish an exact relationship between chemical-catalyst interactions and catalyst parameters, which will allow calculation of these interactions and thus advance their mechanistic understanding.

Elemental two-dimensional nanosheets beyond graphene.

The great success of graphene has encouraged the fast development of other two-dimensional (2D) nanosheets, which have attracted extensive attention in different scientific fields encompassing field effect transistors, lithium-ion batteries, and catalysis. With atomic-scale thickness, almost all of the atoms are exposed on the surface, providing an extremely high specific surface area, in conjunction with special physical, chemical, and electronic properties, owing to the quantum confinement effects, which enable their surface phase to be as important as the bulk counterparts. In this review, we have summarized and discussed the recent advancements of 2D nanomaterials beyond graphene, with an emphasis on their basic fundamentals, preparation strategies, and applications.

Engineering the Electrical Conductivity of Lamellar Silver-Doped Cobalt(II) Selenide Nanobelts for Enhanced Oxygen Evolution.

Precisely engineering the electrical conductivity represents a promising strategy to design efficient catalysts towards oxygen evolution reaction (OER). Here, we demonstrate a versatile partial cation exchange method to fabricate lamellar Ag-CoSe nanobelts with controllable conductivity. The electrical conductivity of the materials was significantly enhanced by the addition of Ag cations of less than 1.

A Generic Wet Impregnation Method for Preparing Substrate-Supported Platinum Group Metal and Alloy Nanoparticles with Controlled Particle Morphology.

Mass production of shape-controlled platinum group metal (PGM) and alloy nanoparticles is of high importance for their many fascinating properties in catalysis, electronics, and photonics. Despite of successful demonstrations at milligram scale using wet chemistry syntheses in many fundamental studies, there is still a big gap between the current methods and their real applications due to the complex synthetic procedures, scale-up difficulty, and surface contamination problem of the made particles. Here we report a generic wet impregnation method for facile, surfactant-free, and scalable preparation of nanoparticles of PGMs and their alloys on different substrate materials with controlled particle morphology and clean surface, which bridges the outstanding properties of these nanoparticles to practical important applications.

Engineering the electronic state of a perovskite electrocatalyst for synergistically enhanced oxygen evolution reaction.

A surface hydrogen effect to modulate the pure electronic-state transition in perovskite Ca0.9 Yb0.1 MnO3 synergistically generates a more suitable eg electron filling status and better conductivity.

Metallic nickel nitride nanosheets realizing enhanced electrochemical water oxidation.

Exploring efficient and inexpensive oxygen evolution reaction (OER) electrocatalysts is of great importance for various electrochemical energy storage and conversion technologies. Ni-based electrocatalysts have been actively pursued because of their promising activity and earth abundance. However, the OER efficiency for most of the developed Ni-based electrocatalysts has been intrinsically limited due to their low electrical conductivity and poor active site exposure yield.

Octahedral Pd@Pt1.8Ni core-shell nanocrystals with ultrathin PtNi alloy shells as active catalysts for oxygen reduction reaction.

Forming core-shell and alloy structures offers generally two ways to design efficient Pt-based catalysts for oxygen reduction reaction (ORR). Here, we combined these two strategies and invented a versatile aqueous route to synthesize octahedral Pd@Pt1.8Ni core-shell nanocrystals.

Carbon monoxide in controlling the surface formation of Group VIII metal nanoparticles.

Group VIII metal nanoparticles with variant morphologies were synthesized under a carbon monoxide atmosphere. The important roles of CO in determining the surface formation of growing particles were studied both by experiment and density functional theory (DFT) calculations, which suggest different growth mechanisms for these metals.