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Studying the relationship between quantum coherence and energy is an intriguing and vital subject in quantum thermodynamics. Quantum engine provides an excellent platform to emphasize it. By constructing a bipartite entanglement engine (BEE) model consisting of a single qubit as the target qubit and a two-qubit as the ancilla, we have investigated the influence of quantum coherence of ancilla on work extraction of BEE at length, and analytically calculated the extractable work of BEE for the ancilla with quantum coherence (QC). We found that the extractable work of BEE is not only dependent on coherence magnitude but also related to the coherence phase of ancilla. Moreover, under certain coherent parameters, the QC can boost the work extraction from BEE. The study reveals the role of QC acting as “fuel” of engine well which deepens the understanding of the energetic effect of QC.

Tailoring the selectivity at the electrode‐electrolyte interface is one of the greatest challenges for heterogeneous electrocatalysis, and complementary strategies to catalyst structural designs need to be developed. Herein, we proposed a new strategy of controlling the electrocatalytic pathways by lateral adsorbate interaction for the bio‐polyol oxidation. Redox‐innocent 1,1,1,3,3,3‐hexafluoro‐2‐propanol (HFIP) anion possesses the alcoholic property that facilely adsorbs on the nickel oxyhydroxide catalyst, but is resistant to oxidation due to the electron‐withdrawing trifluoromethyl groups. The alien HFIP adsorbents can compete with bio‐polyols and form a mixed adsorbate layer that creates lateral adsorbate interaction via hydrogen bonding, which achieved a >2‐fold enhancement of the oxalate selectivity to 55 % for the representative glycerol oxidation and can be extended to various bio‐polyol substrates. Through in situ spectroscopic analysis and DFT calculation on the glycerol oxidation, we reveal that the hydrogen‐bonded adsorbate interaction can effectively tune the adsorption energies and tailor the oxidation capabilities toward the targeted products. This work offers an additional perspective of tuning electrocatalytic reactions via introducing redox‐innocent adsorbates to create lateral adsorbate interactions. [ABSTRACT FROM AUTHOR]

Sodium‐ion batteries (SIBs), based on hard carbon anodes and Na+‐intercalation compound cathodes, have gained significant attention. Nonetheless, hard carbon anodes involve the storage of Na+ at a low potential, typically below 0.1 V (vs Na/Na+), which increases the risk of dendritic Na growth on the anode surface during overcharging. Herein, a safe organic/inorganic composite anode containing tetrasodium 3,4,9,10‐perylenetetracarboxylate (Na4PTC) and Metallic bismuth (Bi) with a weight ratio of 7:2, which exhibits an average potential of 0.7 V (vs Na+/Na) and a capacity of 150 mAh g−1 is proposed. The electrode reaction involves a reversible coordination reaction within the organic host and alloying reactions within the metallic Bi component. Importantly, the organic component efficiently buffers the volume changes in Bi during the alloying reaction, while the metallic Bi enhances the electronic conductivity of the organic material. As a result, this composite anode shows high cycle stability and rate performance, even under high mass loadings ranging from 10 to 50 mg cm−2. Furthermore, it is demonstrated that the Na‐ion full cell, consisting of the composite anode and the Na3V2O2(PO4)2F cathode, exhibits minimal capacity degradation over 100 cycles while maintaining a high areal capacity of 1.1 mA cm−2. [ABSTRACT FROM AUTHOR]

Tailoring the selectivity at the electrode-electrolyte interface is one of the greatest challenges for heterogeneous electrocatalysis, and complementary strategies to catalyst structural designs need to be developed. Herein, we proposed a new strategy of controlling the electrocatalytic pathways by lateral adsorbate interaction for the bio-polyol oxidation. Redox-innocent 1,1,1,3,3,3-hexafluoro-2-propanol (HFIP) anion possesses the alcoholic property that facilely adsorbs on the nickel oxyhydroxide catalyst, but is resistant to oxidation due to the electron-withdrawing trifluoromethyl groups. The alien HFIP adsorbents can compete with bio-polyols and form a mixed adsorbate layer that creates lateral adsorbate interaction via hydrogen bonding, which achieved a >2-fold enhancement of the oxalate selectivity to 55 % for the representative glycerol oxidation and can be extended to various bio-polyol substrates. Through in situ spectroscopic analysis and DFT calculation on the glycerol oxidation, we reveal that the hydrogen-bonded adsorbate interaction can effectively tune the adsorption energies and tailor the oxidation capabilities toward the targeted products. This work offers an additional perspective of tuning electrocatalytic reactions via introducing redox-innocent adsorbates to create lateral adsorbate interactions., (© 2024 Wiley-VCH GmbH.)

Maximizing the loadings of active centers without aggregation for a supported catalyst is a grand challenge but essential for achieving high gravimetric catalytic activity, especially toward multi-step reactions. The oxidation of 5-hydroxymethylfurfural (HMF), a key biomass-derived platform molecule, into 2,5-furandicarboxylic acid (FDCA), a promising alternative to polyester monomer, is such a multi-step reaction that involves 6 proton and electron transfers. This process often demands strong alkaline environment but also suffers from the alkali-driven polymerization side-reaction. Meanwhile, neutral media ameliorates the polymerization, but lacks efficient catalyst toward deep oxidation. Herein, we devised a strategy of creating ultra-dense supported Ru oxide clusters via directed ion exchange in a Co hydroxyanion (CoHA) support material. Pyrimidine ligands were first incorporated into the CoHA interlayers, and the subsequent evacuation of pyrimidines created porous channels for the directed ion exchange with the built-in anions in CoHA, which allowed the dense and mono-disperse functionalization of RuCl 6 2- anions and their resulting Ru oxide clusters. These ultra-dense Ru oxide clusters not only enable high HMF electrooxidation currents under neutral conditions but also create microscopic channels in-between the clusters for the expedited re-adsorption and oxidation of intermediates toward highly oxidized product, such as 5-formyl-2-furoic acid (FFCA) and FDCA. A two-stage HMF oxidation process, consisting of ambient conversion of HMF into FFCA and FFCA oxidation into FDCA under 60 °C, was eventually developed to first achieve a high FDCA yield of 92.1 % under neutral media with significantly reduced polymerization., (© 2024 Wiley-VCH GmbH.)

The electro-reforming of glycerol is an emerging technology of simultaneous hydrogen production and biomass valorization. However, its complex reaction network and limited catalyst tunability restrict the precise steering toward high selectivity. Herein, we incorporated the chelating phenanthrolines into the bulk nickel hydroxide and tuned the electronic properties by installing functional groups, yielding tunable selectivity toward formate (max 92.7 %) and oxalate (max 45.3 %) with almost linear correlation with the Hammett parameters. Further combinatory study of intermediate analysis and various spectroscopic techniques revealed the electronic effect of tailoring the valence band that balances between C-C cleavage and oxidation through the key glycolaldehyde intermediate. A two-electrode electro-reforming setup using the 5-nitro-1,10-phenanthroline-nickel hydroxide catalyst was further established to convert crude glycerol into pure H 2 and isolable sodium oxalate with high efficiency., (© 2023 Wiley-VCH GmbH.)