Yunhua Li

Electrocatalytic propylene oxidation to 1,2‐propylene glycol (PG) offers advantages over thermocatalytic routes through milder reaction conditions and concomitant green hydrogen production. Diverging from conventional palladium oxide paradigms, for the first time we demonstrate hollow nanosphere Pd ₁₇ Se ₁₅ and Pd ₇ Se ₄ exhibiting phase‐dependent reactivity for propylene electrooxidation to PG. Pd ₁₇ Se ₁₅ presents superior selectivity and Faradaic efficiency for PG compared to Pd ₇ Se ₄ and achieves twice the PG Faradaic efficiency of commercial Pd/C, owing to its distinctive crystal phase and local coordination environments. In situ attenuated total reflection Fourier transform infrared spectroscopy with isotopic labeling reveals that enhanced performance originates from optimized propylene adsorption energetics and accelerated *OH generation via efficient water activation. Density functional theory calculations confirm that Pd ₁₇ Se ₁₅ facilitates propylene adsorption and exhibits lower energy barriers for sequential hydroxylation than Pd ₇ Se ₄ . This study establishes the Pd‐Se phase‐dependent correlation in propylene electrooxidation to PG and advances the sustainable electrochemical upgrading strategy of light olefins.

Breaking the activity‐stability trade‐off in acidic oxygen evolution reaction (OER) is pivotal for realizing industrial‐grade proton exchange membrane water electrolyzers (PEMWEs). Herein, we report amorphous/crystalline Ru _0.3 Ir _0.7 O _x nanorods (a/c‐Ru _0.3 Ir _0.7 O _x NRs) synthesized via ion exchange and thermal annealing. The a/c‐Ru _0.3 Ir _0.7 O _x NRs showed a 229 mV overpotential at 10 mA/cm ² . In PEMWEs, the catalyst achieved cell voltages of 1.56 and 1.77 V at 1.0 and 3.0 A/cm ² , respectively, and demonstrated stable operation for 350 h at 1.0 A/cm ² , outperforming most previous reports. Characterization reveals RuO ₂ in crystalline microdomains and IrO ₓ in amorphous regions. In situ studies clearly showed that the OER on a/c‐Ru _0.3 Ir _0.7 O _x NRs proceeds via a hybrid mechanism combining lattice oxygen oxidation (LOM) and adsorbate evolution mechanism (AEM), avoiding the disadvantages of the exclusive LOM and AEM pathways in amorphous (a‐Ru _0.3 Ir _0.7 O _x NRs) and crystalline (c‐Ru _0.3 Ir _0.7 O _x NRs) counterparts and facilitating practical PEMWE application.

The optimized composition and precisely tailored structure configuration play critical roles in enhancing the catalytic reaction kinetics. Here we report a distinctive core@satellite strategy for designing the advanced platinum-nickel@platinum-nickel-copper-cobalt-indium high-entropy alloy nanowires (Pt₃Ni@HEA NWs) as efficient bifunctional catalysts in the proton exchange membrane fuel cell. Impressively, the Pt₃Ni@HEA NWs/C shows 19.4/15.3 times higher mass/specific activity than that of commercial Pt/C for the oxygen reduction reaction. More importantly, synchronously as the cathodic and anodic catalysts, it can achieve a high membrane electrode assembly power density of 1653.5 mW cm^-2 and long-term stability (only 3.9% voltage loss) for 280 h, largely outperforming those of commercial Pt/C. The weakened Pt-CO binding strength, quick removal of CO with linear adsorption, and favorable CO adsorption form contribute to the high performance of Pt₃Ni@HEA NWs/C. This core@satellite strategy provides a new paradigm to develop the comprehensively efficient Pt-based functional catalysts for fuel cells and beyond.

Alcohol electrooxidation is pivotal for a sustainable energy economy. However, designing efficient electrocatalysts for this process is still a formidable challenge. Herein, palladium–selenium nanowires featuring distinct crystal phases: monoclinic Pd ₇ Se ₂ and tetragonal Pd _4.5 Se for ethylene glycol electrooxidation reaction (EGOR) are synthesized. Notably, the supported monoclinic Pd ₇ Se ₂ nanowires ( m ‐Pd ₇ Se ₂ NWs/C) exhibit superior EGOR activity, achieving a mass activity (MA) and specific activity (SA) of 10.4 A mg _Pd ⁻¹ (18.7 mA cm ⁻² ), which are 8.0 (6.7) and 10.4 (8.2) times versus the tetragonal Pd _4.5 Se and commercial Pd/C and surpass those reported in the literature. Furthermore, m ‐Pd ₇ Se ₂ NWs/C displays robust catalytic activity for other alcohol electrooxidation. Comprehensive characterization and density functional theory (DFT) calculations reveal that the enhanced electrocatalytic performance is attributed to the increased formation of Pd ⁰ on the high‐index facets of the m ‐Pd ₇ Se ₂ NWs, which lowers the energy barriers for the C─C bond dissociation in CHOHCHOH* and the CO* oxidation to CO ₂ *. This study provides palladium‐based alloy electrocatalysts exhibiting the highest mass activity reported to date for the electrooxidation of ethylene glycol, achieved through the crystalline phase engineering strategy.

Exploring high-efficiency, robust and cost-efficient anode catalysts for direct methanol fuel cells (DMFCs) is extremely urgent and challenging. Here we report a rational design of hierarchically structured platinum–nickel@platinum–tin core@shell nanowires (H-PtNi@PtSn NWs) for efficient methanol oxidation reaction (MOR) and membrane electrode assembly (MEA) catalysis in DMFCs. In particular, the H-PtNi@PtSn NWs demonstrate exceptional mass and specific activities of 3.35 A mg_Pt ⁻¹ and 3.42 mA cm⁻² for the MOR, along with high stability with limited 18.5% mass activity decay after nine consecutive chronoamperometry cycles for 18 000 s. More importantly, they can realize a MEA power density of 65.1 mW cm⁻² in a single DMFC, better than those of commercial Pt/C and many other reported Pt-based catalysts, revealing promising device application potential. The integration of advantageous hierarchical configuration and the unique core@shell structure effectively avoids the inherent issues of traditional PtNi nanostructures such as limited active sites and poor CO-tolerance. The in situ Fourier transform infrared spectroscopy and CO-stripping measurements collectively reveal that the H-PtNi@PtSn NWs can weaken the chemisorption of the adsorbed CO intermediate and promote its oxidation removal, simultaneously encouraging the “CO free” pathway, thereby boosting the MOR performance and achieving efficient MEA catalysis for DMFCs.

Electrochemical carbon monoxide reduction reaction (CORR) is a potential way to obtain high‐value multi‐carbon (C₂₊) products. However, achieving high selectivity to acetate is still a challenge. Herein, we develop a two‐dimensional Ag‐modified Cu metal–organic framework (Ag_0.10@CuMOF‐74) that demonstrates Faradaic efficiency (FE) for C₂₊ products up to 90.4 % at 200 mA cm⁻² and an acetate FE of 61.1 % with a partial current density of 122.2 mA cm⁻². Detailed investigations show that the introduction of Ag on CuMOF‐74 favors the generation of abundant Cu−Ag interface sites. In situ attenuated total reflection surface enhanced infrared absorption spectroscopy confirms that these Cu−Ag interface sites improve the coverage of *CO and *CHO and the coupling between each other and stabilize key intermediates *OCCHO and *OCCH₂, thus significantly promoting to the acetate selectivity on Ag_0.10@CuMOF‐74. This work provides a high‐efficiency pathway for CORR to C₂₊ products.

The electroreduction of carbon dioxide into high-value-added products is an effective approach to alleviating the energy crisis and pollution issues. However, there are still significant challenges for multicarbon (C₂₊) product production due to the lack of efficient catalysts with high selectivity. Herein, a Cu-rich electrocatalyst, where Cu₂O nanoparticles are decorated on two-dimensional (2D) Cu-BDC metal-organic frameworks (MOFs) with abundant heterogeneous interfaces, is synthesized for highly selective CO₂ electroreduction into C₂₊ products. A high C₂₊ Faradaic efficiency of 72.1% in an H-type cell and 58.2% in a flow cell are obtained, respectively. The heterogeneous interfaces of Cu₂O/Cu-BDC can optimize the adsorption energy of reaction intermediates during CO₂ electroreduction. An in situ infrared spectroscopy study indicates that the constructed interfaces can maintain the particular distribution of Cu valence states, where the C-C coupling is promoted to efficiently produce C₂₊ products owing to the stabilization of *CHO and *COH intermediates.

The selective introduction of Ir changes the electronic structure and optimizes the balanced adsorption of H and OH, making the ultrafine Pt₂Ir distorted nanowire one of the best HER/HOR catalysts reported to date.