Energy & Environmental Science最新文献

Triethyl phosphate (TEP) electrolytes hold significant promise for high-safety lithium metal batteries (LMBs) due to their eco-friendliness and intrinsic nonflammability. However, parasitic reactions with lithium metal, coupled with sluggish reaction kinetics, hinder their practical deployment in LMBs. Hence, we propose a sustainable TEP-based localized high-concentration electrolyte (LHCE) by molecularly regulating the coordination ability and reduction chemistry of anisole diluents, thereby simultaneously overcoming the thermodynamic and kinetic limitations associated with high-concentration electrolytes and conventional LHCEs. The optimized p-methylanisole (pMA) diluent modulates Li–TEP coordination and facilitates anions to enter primary solvation sheath through H^δ+–O^δ− hydrogen-bonding interactions, while the weak ion–dipole interaction between Li⁺ and pMA promotes pMA participation in interfacial reactions and preserves the cation-hopping transport mechanism. This strategy yields robust LiF/Li₂O-rich interphases and accelerates reaction kinetics, enabling lithium metal to achieve a high average coulombic efficiency of 98.7% over 650 cycles and an ultralong-lifespan exceeding 1600 h. When deployed in LMBs paired with 2.5 mAh cm⁻² sulfurized polyacrylonitrile cathodes, the batteries demonstrate an extended lifespan over 600 cycles with an average capacity decay of only 0.03% per cycle. Furthermore, the molecular-level design of diluents is broadly applicable to other alkali–metal batteries, offering a new pathway toward the development of high-energy LMBs.

Despite decades of research on CO₂ capture and conversion, translating laboratory advances into products for widespread public use remains elusive. This review argues that the persistent emphasis on incremental innovations in capture and catalytic conversion overlooks the fundamental barriers that eventually determine large-scale feasibility. Here, we identify and critically evaluate six key bottlenecks that demand urgent attention: (i) the high energy requirement for CO₂ capture and regeneration, (ii) limited efficiency and selectivity of catalytic systems, (iii) infrastructure and scalability constraints, (iv) challenges linked with CO₂ purity and transportations, (v) uncertainties in lifecycle emissions and net carbon reduction, and (vi) inadequate economic incentives and market viability. Significantly, our analysis extends beyond laboratory studies to systematically assess insights from emerging CO₂ capture startups and ongoing commercial ventures, including those in space and defense. By interlinking the technological, infrastructural, and market-based gaps, we demonstrate that progress cannot be measured solely by energy efficiency and productivity; it must instead address the broader ecosystem of deployment questions. To facilitate broader understanding, authors present complex issues through simplified flowcharts and conceptual diagrams, making the debate accessible to scientists, policymakers, and the wider public. Finally, we propose potential paths to overcome these fences, reframing the CCU discussion from “can it be done?” to “what will it take to deploy it?”. In this way, our review provides not only a censorious diagnosis of why commercialization lags but also a framework to guide future research, investment, and policy toward actionable climate solutions.

The application of medium-/high-entropy materials has revolutionized the design of solid-state electrolytes (SSEs) by stabilizing single-phase solutions from otherwise incompatible elements. However, navigating the vast compositional space of entropy-stabilized materials remains a significant challenge. To overcome this, we introduce a machine learning (ML)-accelerated approach to identify multi-cation NASICON oxide SSEs. By training a Gaussian Naive Bayes model on four key descriptors (ionic radius, electronegativity, valence state, and configurational entropy), we found four promising compositions incorporating Zr, Ti, Hf, Lu, Ga, and Sc. These compositions exhibit notable entropy-driven stabilization, demonstrated by the complete suppression of Na₃PO₄/ZrO₂ impurity formation. Among them, the medium-entropy phase Na_3.5Zr_1.0Ti_0.5Lu_0.5Si₂PO₁₂ achieved remarkable performance, delivering an ionic conductivity of 1.3 mS cm⁻¹ at room temperature, a critical current density of 1.9 mA cm⁻², and over 10 000 hours of stable Na plating/stripping. When integrated into all-solid-state sodium batteries with a high-voltage Na₃V₂(PO₄)₂F₃ cathode and a sodium anode, it further demonstrated exceptional battery performance indicators, including high-rate capability (110 mAh g⁻¹ at 5C) and long-term cycling stability (80% capacity retention after 700 cycles at 2C). This work establishes entropy engineering, coupled with ML guidance, as a powerful paradigm for the rational design of next-generation SSEs.

Monolithic all-perovskite tandem solar cells based on mixed cation lead–tin (Pb–Sn) have advanced rapidly in recent years. However, the presence of a considerable amount of volatile methylammonium (MA) adversely constrains the stability of solar devices. Here, we first quantitatively evaluated the thermal stability of Pb–Sn perovskite films containing different types of A-site cations. In comparison to the all-MA and MA–FA binary counterparts, all-formamidinium (FA) Pb–Sn films exhibit the highest decomposition activation energy of 149.13 kJ mol⁻¹. On this basis, high-quality all-FA Pb–Sn perovskite films are prepared by blade coating with addition of a small amount of hydrazinium dichloride (HDC) to the perovskite precursor. The selectively strong coordination of HDC with Sn²⁺ ions not only suppresses the oxidation of Sn²⁺ but, more importantly, balances the nucleation of the Sn- and Pb-based species, resulting in perovskite films with markedly improved homogeneity of the Pb–Sn alloyed phase. The prepared single-junction all-FA Pb–Sn PSCs and MA-free tandem devices yield champion efficiencies of 21.81% and 27.40%, respectively. Moreover, the unencapsulated all-FA Pb–Sn devices retain >80% of their initial efficiencies following 190 h of thermal stress at 85 °C.

The applications of Zn–I₂ batteries are plagued by severe side reactions, including the polyiodide shuttle on the cathode and parasitic by-products on the zinc anode. Herein, we introduce an amino acid derivative, D-penicillamine (DPL), as a molecular-level mediator to simultaneously resolve these challenges. Its functional groups effectively anchor iodine species and catalyze polyiodide conversion, thus suppressing the shuttle effect for highly reversible iodine redox. Concurrently, its preferential adsorption and favorable electronic structure enable the protection of the zinc anode, which inhibits dendrite growth and the gas evolution reaction. Consequently, the DPL-containing electrolyte enables exceptional long-term stability: a symmetric Zn‖Zn cell operates stably for over 1500 h at 5 mA cm⁻² and 1 mAh cm⁻², while a full Zn–I₂ cell endures unprecedented 12 000 cycles at 10 A g⁻¹ with 87.6% capacity retention. In particular at a high I₂ loading of 14.7 mg cm⁻², the corresponding pouch cell exhibits an impressive reversible capacity of 160 mA h g⁻¹ and a considerable retention ratio of 95.2% after 100 cycles at a low current density of 0.5 A g⁻¹. This paper demonstrates that employing molecular mediators is a powerful strategy to design and develop high-performance Zn–I₂ batteries.

Aqueous alkaline nickel-based batteries are regarded as ideal candidates for large-scale energy storage due to their high safety and inherent low cost, but they are plagued by the toxicity, side reactions and high cost of conventional metal anode materials, such as Cd, Zn, and metal hydride alloys. Herein, we report an azo-linked conjugated organic polymer (PBPA) synthesised via in situ electrochemical reduction and coupling of nitro groups on 2,8,14-trinitrohexaazatrinaphthalene (HATN-3NO₂) in a high-concentration alkaline electrolyte with low free water activity. This resulting polymer, featuring a high density of active CN and NN groups and enhanced electron delocalization, emerges as a promising anode owing to its low cost, excellent cyclability, and low redox potential. When assembled into a PBPA//Ni(OH)₂ full cell, it demonstrates remarkable performance, including a high anode-specific capacity of 324.9 mAh g⁻¹, exceptional durability over 30 000 cycles at 10 A g⁻¹, and outstanding low-temperature capabilities (117% capacity retention after 560 cycles at −60 °C), which outperform commercial nickel–hydrogen batteries and most reported aqueous alkaline systems. This potential is further highlighted by the fabrication of a high-mass loading (14.4 mg cm⁻²) self-supporting electrode, which delivers a high operating voltage of 1.25 V with minimal capacity decay, underscoring the significant promise of this system for practical energy storage applications.

Wide-bandgap (WBG) perovskite solar cells (PSCs) serve as essential top cells in perovskite/organic tandem solar cells (POTSCs), where their optoelectronic properties profoundly impact the overall device performance. However, WBG PSCs with high bromine content suffer from substantial energy losses due to inferior film crystallinity and severe phase segregation, which hinder the advancement of efficient POTSCs. Herein, propanedioic acid (PPDA) is designed and adopted as a crystallization regulator to modulate the nucleation and crystal growth kinetics of 1.85 eV WBG perovskites. This strategy enhances film crystallinity and effectively suppresses phase segregation. Additionally, PPDA strengthens field-effect coupling at the perovskite surface through hydrogen bonding with the upper interlayer of propane-1,3-diammonium iodide (PDAI₂), thereby significantly reducing the interfacial non-radiative voltage loss. Consequently, the 1.85 eV WBG PSC achieves an exceptional power conversion efficiency (PCE) of 19.35% and an open-circuit voltage (V_OC) of 1.38 V, along with great operational stability. When integrated with organic sub-cells in a two-terminal tandem configuration, the POTSC delivers an impressive PCE of 26.25% and a notable V_OC of 2.22 V. This work elucidates a synergistic mechanism for simultaneous crystallization regulation and interface enhancement in perovskite photovoltaics, providing valuable insights for developing high-performance WBG PSCs and tandem devices.

Aqueous poly(3,4-ethylenedioxythiophene):polystyrenesulfonate (PEDOT:PSS) solution, universally employed on the interconnection layer (ICL) in all-perovskite and perovskite/organic tandem cells, has the intrinsic risk of perovskite instability induced by moisture erosion. Here we identify the root cause of instabilities caused by conventional PEDOT:PSS. Moisture from the aqueous formulation penetrates downward through the ICL during device fabrication, chemically degrading the underlying wide-bandgap perovskite and irreversibly reducing device efficiency and stability. We replaced PEDOT:PSS with an isopropanol (IPA)-dispersible PEDOT. This stable hole transport material eliminates moisture-induced damage while maintaining uniform, non-destructive coverage on the ICL, effectively resolving the long-standing limitations of aqueous PEDOT:PSS. In addition, the introduction of IPA-dispersible PEDOT reduces buried interfacial recombination in the narrow bandgap tin-lead perovskites and improves hole extraction. As a result, all-perovskite tandem cells achieved power conversion efficiencies of 29.7% (certified 29.6%) and perovskite/organic tandem cells achieved a PCE of 26.5%, and retained 90% of initial performance under continuous 1-sun operation for over 534 hours and 403 h, respectively, demonstrating their universal applicability and reliability for efficient and stable perovskite tandem photovoltaics.

The ever-increasing demand for high-energy rechargeable batteries drives global innovation in new battery chemistry and device design. Here, we propose an asynchronously reverse dual-ion battery (ARDIB) operating with a non-traditional charge storage paradigm that fundamentally differs from existing battery technologies. In this battery, anions and cations are respectively inserted into anode and cathode via an asynchronous process, which was made possible by coupling an insertion-type MnO₂ cathode to accommodate sodium ions (Na⁺) during discharging and a conversion-insertion-type Mg–Y alloy anode for storing hydride ions (H⁻) during charging. This H⁻–Na⁺ ARDIB benefits from an aqueous electrolyte containing tetramethylammonium hydroxide (TMAOH), which triggers microstructural reconstruction of the thick MnO₂ cathode and supports the reversible alloy-hydride conversion of the anode. As a planar micro-battery, the ARDIB delivers a high areal capacity of 0.43 mAh cm⁻² and an energy density of 0.42 mWh cm⁻² at 1 mA cm⁻², maintains stable operation for 5700 cycles at 10 mA cm⁻² and exhibits superior rate capability with a maximum power density of 30.8 mW cm⁻². These performance metrics surpass those of most reported micro-batteries and enable integration with miniature electronic devices and photovoltaic harvesting systems, providing a configuration-based solution for next-generation energy storage.