Carbon Energy最新文献

Cement occupies a significant proportion in construction, serving as the primary material for components such as bricks and walls. However, its role is largely limited to load-bearing functions, with little exploration of additional applications. Simultaneously, buildings remain a major contributor to global energy consumption, accounting for 40% of total energy use. Here, we for the first time endow cement with energy storage functionality by developing cement-based solid-state energy storage wallboards (CSESWs), which can utilize the ample idle surface areas of building walls to seamlessly store renewable energy from distributed photovoltaics without compromising building safety or requiring additional space. Owing to unprecedented microstructures and composition interactions, these CSESWs not only achieve a superionic conductivity of 101.1 mS cm⁻¹ but also demonstrate multifunctionality, such as significant toughness, thermal insulation, lightweight, and adhesion. When integrated with asymmetrical electrodes, the CSESWs exhibit a remarkable capacitance (2778.9 mF cm⁻²) and high areal energy density (10.8 mWh cm⁻²). Moreover, existing residential buildings renovated with our CSESWs can supply 98% of daily electricity needs, demonstrating their outstanding potential for realizing zero-carbon buildings. This study pioneers the use of cement in energy storage, providing a scalable and cost-effective pathway for sustainable construction.

The global drive for sustainable energy solutions intensified interest in anion exchange membrane water electrolysis (AEMWE), as a promising hydrogen production pathway, leveraging renewable energy sources. However, widespread adoption is hindered by the high cost and non-optimised design of crucial components, such as porous transport layers (PTL) and flow fields. This study comprehensively investigates the interplay between structure, mechanics, and electrochemical performance of a low-cost knitted wire mesh PTL, focusing on its potential to enhance cell assembly and operation. Electrochemical characterisation was performed on a single 4 cm² cell, using 1 M KOH at 60°C. Knitted wire mesh PTL, characterised by approximately 70% porosity, 2 mm thickness, and 1.098 tortuosity, delivered a 33% improvement in current density compared to the standard cell configuration. Introducing a knitted PTL interlayer reduced cell voltage by 74 mV at 2 A cm⁻² by improving compression force distribution across the active area, enhancing gas transport and maintaining optimal electrical and thermal conductivity. These findings highlight the significant potential of innovative PTL designs in AEMWE to improve mechanical and operational efficiency without increasing the cost.

The development of formic acid dehydrogenation materials with high activity and low cost is key to realizing hydrogen energy utilization. Herein, we describe a specific low-loading strategy to construct a high-activity Co atom site catalyst for this reaction. Under optimal conditions, the formic acid dehydrogenation performance of Co─Fe dual-atom catalyst (turnover frequency of 2,446.8 h⁻¹, hydrogen production rate of 1,015,306.1 mL g_Co⁻¹ h⁻¹) was 300 times greater than that of commercial 5% Pd/C. High-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure spectra, combined with theoretical calculations, confirm that the presence of different active sites (Co single-atom, Co–Co dual-atom, Co─Fe dual-atom) in catalysts is the key factor affecting their catalytic activity. These findings provide a strong scientific basis for the development of single-atom and dual-atom catalysts.

Acidic environments enhance CO₂ utilization during CO₂ electrolysis via a buffering effect that converts carbonates formed at the electrode surface back into CO₂. Nevertheless, further investigation into acidic CO₂ electrolysis is required to improve its selectivity towards certain CO₂ reduction reaction (CO₂RR) products, such as multicarbon (C₂₊) species, while enhancing its overall stability. In this study, liquid product recirculation in the catholyte and local OH⁻ accumulation were identified as primary factors contributing to the degradation of gas diffusion electrodes mounted in closed-loop catholyte configurations. We demonstrate that a single-pass catholyte configuration prevents liquid product recirculation and maintains a continuous flow of acidic-pH catholyte throughout the reaction while using the same volume as a closed-loop setup. This approach improves electrode durability and maintains a Faradaic efficiency of 67% for multicarbon products over 4 h of CO₂ electrolysis at −600 mA cm⁻².

Back cover image: The exsolution method offers a powerful route for developing efficient and stable electrocatalysts. In article number e70013, Sun et al. present a pnictogenation-assisted exsolution approach to fabricate size-tunable Ru nanocatalysts embedded in a conductive metal pnictogenide matrix. By tuning the pnictogenation conditions, they achieve controlled formation of Ru nanoclusters and single atoms, enabling tailored catalytic performance. The resulting materials exhibit exceptional electrocatalytic performance for the hydrogen evolution reaction, with improved stability and activity attributed to strong interfacial electronic interactions.

Front cover image: Oxygen carriers play pivotal roles in various chemical looping processes, such as CO₂ splitting. Nevertheless, they have been restricted by deactivation and inferior oxygen transferability at low temperatures, and in article number e70011, Sun et al. design a Fe–O_v–Ce-triggered phase-reversible CeO_2−x·Fe·CaO oxygen carrier with strong electron-donating ability, which activates CO₂ at low temperatures and promotes oxygen transformation.

Gel polymer electrolytes (GPEs) with high flame-retardant concentration can remarkably reduce the thermal runaway risk of lithium metal batteries (LMBs). However, higher flame-retardant content in GPEs always leads to increased leakage of active component and severe lithium corrosion, which greatly hinders the service life of LMBs. Herein, GPEs with high-loading triphenyl phosphate (TPP) are originally fabricated by coaxial electrospinning and stabilized by dual confinement effects, including chemisorption of polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP), and physical encapsulation of polyacrylonitrile (PAN)/PVDF-HFP. These effects arise from the strong polar interactions between the −CF₃ group in PVDF-HFP and P=O group in TPP, as well as the superior anti-swelling property of PAN. To mitigate TPP-induced corrosion during cycling, the optimized Li anode is armored with LiF-rich solid electrolyte interphase (SEI) layer through immersing it in fluoroethylene carbonate-containing electrolyte. As expected, the corresponding Li||Li symmetric cells deliver long-term stable cycling behavior over 2400 h at 0.5 mA cm⁻², and the LiFePO₄||Li batteries hold a high-capacity retention ratio of 81.7% after 6000 cycles at 10 C with excellent flame retardancy. These findings offer new insight into designing the SEI layer for lithium metal in flame-retardant electrolytes, thus promoting the development and application of high-security LMBs.

Photoelectrochemistry is a promising method for the direct conversion of sunlight into valuable chemicals by combining the functions of solar panels and electrolyzers in one technology. In most studies, semiconductor/catalyst photoelectrode assemblies are used to achieve reasonable efficiencies. At the same time, unlike in dark electrochemical processes, the role of the catalyst is not straightforward in photoelectrochemistry, where the onset potential of the redox process should be mostly determined by the flatband potential of the semiconductor. In addition, the energy of holes (i.e., the surface potential) is independent of the applied bias; it is defined by the valence band (VB) position. In this study, we compared PdAu, Au, and Ni on Si photoanodes in the photoelectrochemical (PEC) oxidation of glycerol at record high current densities (> 180 mA cm^‒2), coupled to H₂ evolution at the cathode. We successfully decreased the energy requirement (i.e., the cell voltage) of the paired conversion of glycerol and water by 0.7 V by exchanging the widely studied Ni catalyst with PdAu. The catalyst choice also dictates the product distribution, resulting mainly in C3 products on PdAu, glycolate (C2 product) on Au, and formate (C1 product) on Ni, without complete mineralization of glycerol (CO₂ formation) that is difficult to rule out in dark electrochemical processes (as demonstrated by comparative measurements). Finally, we achieved a bias-free (standalone) operation with PdAu/Si and Au/Si photoanodes by combining the PEC oxidation of glycerol with oxygen reduction reaction (ORR).

The design of efficient and cost-effective bifunctional catalysts, which are capable of driving both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), is of paramount importance for advancing overall water splitting. Here, we developed an innovative heterogeneous interface engineering strategy to boost the electrocatalytic performance of overall water splitting. This approach involves the synergistic integration of ultra-fine CoMoP nanocrystals coupled with three-dimensional (3D) porous C₃N₄/N-doped carbon (NC) architectures, constructing a distinctive CoMoP/C₃N₄/NC heterogeneous interface. The CoMoP/C₃N₄/NC exhibits distinguished overall water splitting performance. To drive the overall water splitting current of 10 mA cm⁻², the CoMoP/C₃N₄/NC||CoMoP/C₃N₄/NC electrolysis cell only needs an ultralow cell voltage of 1.496 V. The electronic properties and localized coordination environments characterizations, and density functional theory (DFT) calculations elucidate that the improved catalytic activities of CoMoP/C₃N₄/NC are primarily attributed to the synergistic interfacial coupling between CoMoP/C₃N₄/NC heterogeneous interface. A novel multi-site synergistic catalytic mechanism was revealed by the DFT calculations, in which the optimum H* adsorption site on CoMoP/C₃N₄/NC for HER is on the cobalt atoms in CoMoP with the ultralow Gibbs free energy of hydrogen bonding (ΔG_H*) of 0.018 eV, while for the OER, the optimum intermediates adsorption site of the CoMoP/C₃N₄/NC is on the carbon atoms in C₃N₄/NC. Besides, the intricately engineered 3D hierarchical porous framework of the CoMoP/C₃N₄/NC can facilitate the ion and electron transport and improve mass transfer, which gives rise to enhanced water splitting performance.

The practical application of lithium (Li) metal batteries (LMBs) faces challenges due to the irreversible Li deposition/dissolution process, which promotes Li dendrite growth with severe parasitic reactions during cycling. To address these issues, achieving uniform Li-ion flux and improving Li-ion conductivity of the separator are the top priorities. Herein, a separator (PCELS) with enhanced Li-ion conductivity, composed of polymer, ceramic, and electrically conductive carbon, is proposed to facilitate fast Li-ion transport kinetics and increase Li deposition uniformity of the LMBs. The PCELS immobilizes PF₆^– anions with high adsorption energies, leading to a high Li-ion transference number. Simultaneously, the PCELS shows excellent electrolyte wettability on both its sides, promoting rapid ion transport. Moreover, the electrically conductive carbon within the PCELS provides additional electron transport channels, enabling efficient charge transfer and uniform Li-ion flux. With these advantages, the PCELS achieves rapid Li-ion transport kinetics and uniform Li deposition, demonstrating excellent cycling stability over 100 cycles at a high current density of 12.0 mA cm^–2. Furthermore, the PCELS shows stable cycling performances in Li–S cell tests and delivers an excellent capacity retention of 95.45% in the Li|LiFePO₄ full-cell test with a high areal capacity of over 5.5 mAh cm^–2.