Yu Wang

All-solid-state lithium-sulfur batteries promise high specific energy and low cost. However, they are challenged by poor rate capability and cycling stability owing to the slow solid-solid sulfur redox reactions. Here, we present fast-charging and durable all-solid-state lithium-sulfur batteries enabled by a pre-embedded solid-solid redox mediator using an amorphous sulfur/iodine nano-eutectic positive electrode. The iodine, intimately homogenized with sulfur owing to carbon mesopore encapsulation, undergoes rapid I₂/I⁻ redox reaction, mediating solid-solid sulfur reactions by promoting electron transfer across the boundaries. The iodine within the carbon and on its surface reacts in situ with the sulfide catholyte to form a globally distributed I₂/I⁻ nano-network throughout the positive electrode, thereby enabling fast charging. The cell exhibits a specific capacity of 851.9 mA h g⁻¹_S/I when charged at 10 C, and 474.7 mA h g⁻¹_S/I at a charging rate of 24 C (1 C is defined as 945 mA g⁻¹_S/I). The high reversibility of the redox-mediated reaction enables durable cycling for 9,000 cycles over 9 months at 2 C and 2,800 cycles over 17 months at 0.5 C. This strategy represents a perspective for developing solid-state conversion electrodes that are plagued by sluggish reactions.

Dissolution of ruthenium (Ru) species under harsh anode operating conditions severely impedes the commercialization of non–iridium (Ir) proton exchange membrane water electrolyzers (PEMWEs). Here, we propose a catalyst design strategy that engineers phases beyond conventional atomic ordering, constructing a heterophase MoRuO _x catalyst (AC-MoRuO _x ). This catalyst achieves 10 milliamperes per square centimeter in an acidic oxygen evolution reaction with merely 180-millivolt overpotential while operating stably for >3000 hours. In PEMWE devices, AC-MoRuO _x delivers record durability at industrial current densities: ≥2000 hours at 1.0 ampere per square centimeter and 1000 hours at 1.5 amperes per square centimeter. We demonstrate that heterophase architecture and atomic arrangements reconfigure electronic structures and phase distribution, simultaneously optimizing active-site density and structural integrity. This breakthrough resolves the long-standing activity-stability trade-off in ruthenium-based catalysts.

Selective production of valuable glycerol chemicals, such as glycerate (which serves as an important chemical intermediate), poses a significant challenge due to the facile cleavage of C–C bonds and the presence of multiple reaction pathways. This challenge is more severe in the electro-oxidation of glycerol, which requires the development of desirable electrocatalysts. To facilitate the glycerol electro-oxidation reaction to glycerate, here we present an approach utilizing a high-entropy PtCuCoNiMn nanosurface. It exhibits exceptional activity (~200 mA cm⁻² at 0.75 V versus a reversible hydrogen electrode) and selectivity (75.2%). In situ vibrational measurements and theoretical calculations reveal that the exceptional glycerol electro-oxidation selectivity and activity can be attributed to the unique characteristics of the high-entropy surface, which effectively modifies the electronic structure of the exposed Pt sites. The catalyst is successfully applied in an electrolyser for long-term glycerol electro-oxidation reaction, demonstrating excellent performance (~200 mA cm⁻² at 1.2V_cell) over 210 h. The present study highlights that tailoring the catalytic sites at the catalyst–electrolyte interface by constructing a high-entropy surface is an effective strategy for electrochemical catalysis.

Ligand advancements have propelled the development of sophisticated ligand strategies for nanocatalysis. These strategies offer the tantalizing prospect of nanoparticles to achieve remarkable selectivity for catalytic process. However, achieving electronic/steric control and realizing selectivity regulation in nanocatalysis remains a formidable challenge, as the dynamic nature of metal-ligand interfaces, including dissolution and structural reconstruction, poses significant obstacles. Herein, we disclose carboranyls (CBs) as carbon-bonded global vertexes coordinating ligands (E_{ads.c−Au(111)} = -2.90 eV, E_{ads.BHs−Au(111)} = -0.54 eV) for gold nanoparticles (AuNPs), showcasing their exceptional inherent stabilization capability and the unique core (Au_n)-satellite (CB₂Au⁻) structure of the resulting NPs. Leveraging these distinct features, CB@AuNPs accomplished regio-selective bromination of aromatic feedstocks including chlorobenzene (p:o > 30:1) and phenyl acrylate, a prominent transformation in chemical industry suffered from selectivity issue. Systematic investigations unveiled the advantages of CB@AuNPs, including: 1) the global coordinating capability of ligands in their vicinity, and 2) the presence of inert counterions. These characteristics enable selectivity regulation through counterion manipulation and harness the substituent effect arising from the stabilized catalytic micro-environment at nanoscale. The effective control of regio-selectivity achieved through the global coordination of carboranyls offers valuable insights into expanding current strategy with heterocatalysts via ligand approach.

The performances of single-atom catalysts are governed by their local coordination environments. Here, a thermal replacement strategy is developed for the synthesis of single-atom catalysts with precisely controlled and adjustable local coordination environments. A series of Co-S_xN_4−x (x = 0, 1, 2, 3) single-atom catalysts are successfully synthesized by thermally replacing coordinated N with S at elevated temperature, and a volcano relationship between coordinations and catalytic performances toward electrochemical CO₂ reduction is observed. The Co-S₁N₃ catalyst has the balanced COOH*and CO* bindings, and thus locates at the apex of the volcano with the highest performance toward electrochemical CO₂ reduction to CO, with the maximum CO Faradaic efficiency of 98 ± 1.8% and high turnover frequency of 4564 h⁻¹ at an overpotential of 410 mV tested in H-cell with CO₂-saturated 0.5 M KHCO₃, surpassing most of the reported single-atom catalysts. This work provides a rational approach to control the local coordination environment of the single-atom catalysts, which is important for further fine-tuning the catalytic performance.

One-step conversion of low-purity polyolefins to value-added products without pretreatments represents a great opportunity for chemical recycling of waste plastics. However, additives, contaminants, and heteroatom-linking polymers tend to be incompatible with catalysts that break down polyolefins. Here, we disclose a reusable, noble metal–free and impurity-tolerant bifunctional catalyst, MoS _x -Hbeta, for hydroconversion of polyolefins into branched liquid alkanes under mild conditions. The catalyst works for a wide scope of polyolefins, including different kinds of high–molecular weight polyolefins, polyolefins mixed with various heteroatom-linking polymers, contaminated polyolefins, and postconsumer polyolefins with/without cleaning under 250°C and 20 to 30 bar H ₂ in 6 to 12 hours. A 96% yield of small alkanes was successfully achieved even at a temperature as low as 180°C. These results demonstrate the great potentials of hydroconversion in practical use of waste plastics as a largely untapped carbon feedstock.

To develop efficient and durable acidic oxygen–reduction–reaction (ORR) catalysts based on all platinum group metals (PGMs) is crucial for large-scale application of proton-exchange membrane fuel cells (PEMFCs) but challenging. Here, we report a nitrogen coordination-induced strong metal–support interaction that can tune the surface atoms of ORR-inactive PGM clusters into efficient and durable active sites. Taking Rh as an example, the carbonization of Rh-overdoped zeolitic imidazolate framework-8 results in a large number of Rh clusters (with a little atomic Rh) in porous nitrogen-doped carbon. The cluster surface atoms coordinate with the nitrogen of the carbon support, forming much stronger metal–support interactions than that of common N-doped carbon-supported metal nanoparticles. The activity of surface-activated Rh clusters is close to that of Pt/C. The regulation rules for the surface active sites inherit most of the characteristics of the corresponding single-atom catalysts, but without their severe instability problem. This surface activation strategy has also shown applicable to other PGMs, thereby it is a promising way to alleviate the reliance of PEMFCs on platinum.

The carbon dioxide and carbon monoxide electroreduction reactions, when powered using low-carbon electricity, offer pathways to the decarbonization of chemical manufacture^1,2. Copper (Cu) is relied on today for carbon–carbon coupling, in which it produces mixtures of more than ten C₂₊ chemicals^3,4,5,6: a long-standing challenge lies in achieving selectivity to a single principal C₂₊ product^7,8,9. Acetate is one such C₂ compound on the path to the large but fossil-derived acetic acid market. Here we pursued dispersing a low concentration of Cu atoms in a host metal to favour the stabilization of ketenes¹⁰—chemical intermediates that are bound in monodentate fashion to the electrocatalyst. We synthesize Cu-in-Ag dilute (about 1 atomic per cent of Cu) alloy materials that we find to be highly selective for acetate electrosynthesis from CO at high *CO coverage, implemented at 10 atm pressure. Operando X-ray absorption spectroscopy indicates in situ-generated Cu clusters consisting of 2+ product¹¹.

Developing active single-atom-catalyst (SAC) for alkaline hydrogen evolution reaction (HER) is a promising solution to lower the green hydrogen cost. However, the correlations are not clear between the chemical environments around the active-sites and their desired catalytic activity. Here we study a group of SACs prepared by anchoring platinum atoms on NiFe-layered-double-hydroxide. While maintaining the homogeneity of the Pt-SACs, various axial ligands (−F, −Cl, −Br, −I, −OH) are employedviaa facile irradiation-impregnation procedure, enabling us to discover definite chemical-environments/performance correlations. Owing to its high first-electron-affinity, chloride chelated Pt-SAC exhibits optimized bindings with hydrogen and hydroxide, which favor the sluggish water dissociation and further promote the alkaline HER. Specifically, it shows high mass-activity of 30.6 A mgPt⁻¹and turnover frequency of 30.3 H₂s⁻¹at 100 mV overpotential, which are significantly higher than those of the state-of-the-art Pt-SACs and commercial Pt/C catalyst. Moreover, high energy efficiency of 80% is obtained for the alkaline water electrolyser assembled using the above catalyst under practical-relevant conditions.