Energy & Environmental Science最新文献

Electrochemical carbon capture offers a sustainable route to mitigate CO₂ emissions, but practical deployment is often limited by modest capture rates and system complexity. Here we report a saline–water electrolysis strategy that simultaneously captures CO₂ and converts it to sodium bicarbonate (NaHCO₃) without external chemical additives. Hydroxide ions (OH⁻) generated in situ at the cathode via the hydrogen-evolution reaction (HER) enable rapid CO₂ absorption and selective conversion to NaHCO₃ by maintaining the catholyte at pH 8–9, consistent with thermodynamic speciation. In simulated flue gas, the system delivers a CO₂ capture rate of 5.27 mmol_CO2 cm⁻² h⁻¹ (55.6 kg_CO2 m⁻² day⁻¹) at 300 mA cm⁻², >99.5% capture efficiency, >90% faradaic efficiency, and energy consumption as low as 87 kJ mol_CO2⁻¹ (1.98 GJ t_CO2⁻¹). The process is tolerant to sulfur dioxide (SO₂), maintaining ∼85% NaHCO₃ conversion for >240 h with 1.0% SO₂ in the feed. Using pure water as the catholyte enables direct production of high-purity NaHCO₃, enhancing operational flexibility. Techno-economic analysis indicates capture costs with US$90.3 per t_CO2 when co-located with a desalination facility and low-cost electricity, while considering the revenues from products NaHCO₃, H₂ and Cl₂ can further improve the economics. This multifunctional, impurity-resistant, and renewable-compatible approach offers a practical, scalable pathway for industrial CO₂ capture and mineralization.

The commercialization of wide-bandgap (WBG) perovskite solar cells (PSCs) faces critical challenges in high-humidity fabrication environments and long-term operational stability. To address these issues, this study introduced 4-mercaptophenylacetic acid (MPAA) as a redox mediator into the perovskite. MPAA facilitates cyclic regeneration through the reversible conversion of thiol-disulfide, simultaneously reducing I₂ and oxidizing Pb⁰, thereby effectively suppressing phase separation. Furthermore, its benzene ring's hydrophobic structure forms moisture barrier, significantly improving the fabrication adaptability of the perovskite in a high-humidity environment. Benefiting from these characteristics, the device fabricated by blade coating in high-humidity ambient air (≈65% relative humidity, RH) achieves a power conversion efficiency (PCE) of 23.16%, which is the state-of-the-art result for the WBG (≥1.68 eV) PSCs fabricated in ambient air. The fabricated mini-module (13 cm²) achieves a PCE of 18.46%, demonstrating the scaling potential of this strategy. Meanwhile, the MPAA-doped device retained 90.2% of its initial PCE after aging for 500 hours under the ISOS-L-3 protocol (85 °C, 50% RH), while the control device exhibited almost complete degradation. This strategy overcomes the limitations of high-humidity fabrication and long-term operational stability problems of WBG PSCs, thus providing significant support for the industrialization of perovskite photovoltaics.

As an emerging sustainable energy technology, moisture-electric generators (MEGs) can spontaneously harvest electricity from ubiquitous water vapor. Natural wood, with its abundant oxygen-containing functional groups and anisotropic microchannels, is an ideal material for MEG fabrication. However, most wood-based generators rely on streaming potential driven by evaporation, requiring an external water supply to ensure continuous operation, which significantly limits their practical applications. Here, we present an asymmetric hygroscopic structure based on delignified natural wood, with LiCl and carbon black incorporated into the hygroscopic and hydrophobic sides, respectively. This design maintains a stable internal water content gradient through the dynamic equilibrium of moisture sorption–desorption, enabling continuous directional ion migration and stable output for over 220 h. Delignification enhances hydrophilicity and surface charge density by exposing cellulose nanofibrils. Additionally, the radiative cooling effect of the hygroscopic layer induced by delignification promotes moisture sorption and prevents the collapse of the water content gradient under solar heating. A single device can continuously generate an open-circuit voltage of ∼0.94 V and a short-circuit current of ∼43 µA at 25 °C and 70% RH, with a maximum output power density of ∼29 µW cm⁻³. This work provides a sustainable strategy for developing efficient bio-based MEGs.

Wide-bandgap perovskites are widely used in tandem solar cells due to their tunable bandgaps (1.5–2.3 eV) enabled by mixed halide compositions. However, significant open-circuit voltage losses persist, especially when the bandgap is increased to ∼1.95 eV with high bromine (Br) content. High Br incorporation often leads to heterogeneous halide distributions within the bulk, resulting in severe phase segregation and enhanced carrier recombination. To address these issues, a halide-mixing braking strategy is employed by introducing potassium cyanate as a halide-mixing “brake”. This approach effectively slows the halide exchange rate during annealing, promoting homogeneous halide distribution throughout the films. Additionally, it improves perovskite film quality by reducing defect densities, thereby suppressing non-radiative recombination losses. As a result, single-junction 1.95 eV-bandgap perovskite solar cells achieved a power conversion efficiency of 15.93%, with a high open-circuit voltage of 1.40 V and a fill factor of 0.83. Furthermore, mechanically stacked triple-junction all-perovskite tandem solar cells employing 1.95, 1.60, and 1.25 eV perovskite light absorbers achieved efficiencies exceeding 30%. Therefore, this work provides a simple and effective strategy for optimizing high-Br-content perovskites, enabling the development of high-efficiency wide-bandgap perovskite and multi-junction tandem solar cells.

Molecular semiconductors have the potential to enable new possibilities in the fields of radiation detection and space applications, but they need to prove resilience against the ionizing radiation present in these harsh environments. The lack of molecular oxygen in space requires the challenging task of performing the degradation studies at inert conditions. In this work, a strategy is presented to investigate the inert radiation hardness of molecular semiconductors using total ionizing dose (TID) tests based on gamma radiation from a cobalt-60 (Co-60) source - a traditional proxy for the space environment. For the first time, a large-scale gamma stability screening of 46 structurally diverse organic semiconductors was performed at inert conditions, deriving a stability target from the UV-visible (UV-vis) evolutions during degradation. The resulting stability ranking of the small-molecule hole transport materials (HTMs) designed for use in perovskite solar cells spans more than two orders of magnitude and shows that molecular structure - rather than atomic composition alone - governs gamma stability. On average, the ionizing dose tolerance exceeds 10 kGy, corresponding to a calculated lifetime of over two years in the Van Allen belt at ∼1000 km altitude in low Earth orbit (LEO). Derivatives of 4,4-difluoro-4-bora-3a,4a-diaza-s-indacene (BODIPY) stand out, even showing seemingly infinite stability targets. Using the ranking, a predictive model could be trained, which implies that the number of boron atoms – or the BODIPY unit in which they are embedded – outperforms more than 1900 other structural and semi-empirical descriptors. Overall, this work lays the groundwork for future gamma stability studies of molecular semiconductors and thin-film technologies in general. With more efforts targeted at understanding the structure-stability relationships and structure-dependent degradation mechanisms, including up to complete recovery of the UV-vis spectra, this class of materials could become a competitive option for ionizing radiation detectors as well as for organic and perovskite space solar cells.

Electrochemical conversion of methane (CH₄) is a sustainable route for converting greenhouse gases into valuable liquid fuels and chemicals. However, achieving high-yield products at industrially relevant current densities remains a formidable challenge. Here, we report a machine learning-guided Mo–Cu dual-site cascade catalytic strategy, enabling selective modulation of key *CH₃O and achieving ethanol (EtOH) electrosynthesis. This system delivers a current density of 103 mA cm⁻² with an EtOH faradaic efficiency of 55.8% ± 0.2%, establishing new performance benchmarks. Mechanistic and DFT analyses reveal that CH₄ is activated by a three-electron *O₂⁻-mediated oxidation pathway, while *CH₃ spillover from Mo to Mo–Cu active sites facilitates exothermic C–C coupling, leading to high-efficiency EtOH production. Techno-economic analysis suggests that integrating renewable electricity can lower the CH₄-to-EtOH production cost from $2.12 per kg to $1.50 per kg within a decade, offering a 53% energy return. This work establishes a cascade-regulated, dual-site framework for efficient CH₄-to-EtOH conversion and offers a framework for machine learning-assisted catalyst design, contributing to cleaner energy technologies and substantial reductions in greenhouse gas emissions.

Zn metal is a suitable anode in aqueous batteries, but it suffers from mossy deposition and side reactions. Herein, we systematically elucidate the kinetically controlled morphology evolution of Zn deposition in the conventional ZnSO₄ electrolyte and accordingly present the 2-methoxyethyl acetate (MA) additive to enable a thermodynamically governed deposition behavior. The unique charge distribution of the MA molecule alters the Zn²⁺ solvation shells in the electrolyte as well as during the desolvation process. It helps with solvation water release to inhibit side reactions, and the controlled final removal of chelated MA leads to the formation of a thermodynamically favored plate morphology. The local enrichment of desolvated MA further shields the unique Zn crystal plane and allows dense packing. As a result, the lifespan of symmetric Zn cells reaches 5740 h after 1.6 vol% MA addition, which is around 8 months and more than 72 times that of the baseline system. With a 50% depth of discharge, the MA additive also extends the cycle life from 40 h to over 1580 h. A Zn//V₆O₁₃·H₂O full cell with an N/P ratio of 1.8 maintains a high capacity of 302 mAh g⁻¹ after 600 cycles at 5 A g⁻¹, superior to only 90 mAh g⁻¹ retained after 250 cycles with the baseline electrolyte.

Breaking the optical symmetry is vital for light-harvesting devices, while the broadband asymmetric light manipulation remains challenging. Herein, optical non-reciprocity with subwavelength pyramid arrays (SPAs) is proposed to synergistically harness the Mie resonance and the multi-order diffraction for blocking light escaping. A forward optical transmittance of over 95% is obtained with an asymmetric ratio of over 2.5 dB in a wide spectral region that fully covers the absorption spectrum of organic solar cells (OSCs). The non-reciprocal optical path in OSCs reduces the threshold thickness of the active layer for efficient light-harvesting as well as the boost in charge extraction. The optimized OSCs achieve an efficiency of 20.70% and a certified value of 19.71%. The versatility of the optical non-reciprocity with SPAs has also been demonstrated for the performance enhancement in perovskite and quantum dot solar cells with different absorption spectra. This strategy surpasses traditional anti-reflective schemes and paves the way for optical manipulation in thin-film optoelectronic devices.