eScience最新文献

Electrocatalytic CO₂ reduction (ECR) to high-value fuels and chemicals offers a promising conversion technology for achieving sustainable carbon cycles. In recent years, although great efforts have been made to develop high-efficiency ECR catalysts, challenges remain in achieving high activity and long durability simultaneously. Taking advantage of the adjustable structure, tunable component, and the M–Ch (M ​= ​Sn, In, Bi, etc., Ch ​= ​S, Se, Te) covalent bonds stabilized metal centers, the p-block metal chalcogenides (PMC) based electrocatalysts have shown great potential in converting CO₂ into CO or formates. In addition, the unique p-block electron structure can suppress the competitive hydrogen evolution reaction and enhance the adsorption of ECR intermediates. Seeking to systematically understand the structure–activity relationship of PMC-based ECR catalysts, this review summarizes the recent advances in designing PMC electrocatalysts for CO₂ reduction based on the fundamental aspects of heterogeneous ECR process, including advanced strategies for optimizing the intrinsic activity and improving the loading density of catalytic sites, constructing highly stable catalysts, and tuning product selectivities. Subsequently, we outline the challenges and perspectives on developing high-performance PMC ECR catalysts for practical applications.

Organic optoelectronic materials enable cutting-edge, low-cost organic photodiodes, including organic solar cells (OSCs) for energy conversion and organic photodetectors (OPDs) for image sensors. The bulk heterojunction (BHJ) structure, derived by blending donor and acceptor materials in a single solution, has dominated in the construction of active layer, but its morphological evolution during film formation poses a great challenge for obtaining an ideal nanoscale morphology to maximize exciton dissociation and minimize nongeminate recombination. Solution sequential deposition (SSD) can deliver favorable p–i–n vertical component distribution with abundant donor/acceptor interfaces and relatively neat donor and acceptor phases near electrodes, making it highly promising for excellent device performance and long-term stability. Focusing on the p–i–n structure, this review provides a systematic retrospect on regulating this morphology in SSD by summarizing solvent selection and additive strategies. These methods have been successfully implemented to achieve well-defined morphology in ternary OSCs, all-polymer solar cells, and OPDs. To provide a practical perspective, comparative studies of device stability with BHJ and SSD film are also discussed, and we review influential progress in blade-coating techniques and large-area modules to shed light on industrial production. Finally, challenging issues are outlined for further research toward eventual commercialization.

Bismuth sulfide (Bi₂S₃) is a dominant anode material for sodium-ion batteries due to its high theoretical capacity. However, extreme volume fluctuations as well as low electrical conductivity and reaction kinetics still limit its practical applications. Herein, we construct an abundant heterointerface of Bi/Bi₂S₃ by engineering the structure of Bi nanoparticles embedded on Bi₂S₃ nanorods (denoted as Bi–Bi₂S₃ NRs) to effectively solve the abovementioned obstacles. Theoretical and systematic characterization results reveal that the constructed heterointerface of Bi/Bi₂S₃ has a built-in electric field, significantly boosts the electrical conductivity, enhances the Na⁺ diffusion kinetics, and buffers the volume variation. With this modification, it can deliver long cycling life, with an ultra-high capacity of 500 mAh g⁻¹ over 500 cycles at 1 ​A ​g⁻¹, and outstanding rate capability, with a capacity of 456 mAh g⁻¹ even at 15 ​A ​g⁻¹. Moreover, a full cell can achieve a high energy density of 180 ​Wh kg⁻¹ at a power density of 40 ​W ​kg⁻¹. Our research opens up a fresh path for improving the dynamics and structural stability of metal sulfide-based electrode materials for SIBs.

The lithium-ion battery (LIB) has enabled portable energy storage, yet increasing societal demands have motivated a new generation of more advanced LIBs. Although the discovery and optimization of battery active materials has been the subject of extensive study since the 1980s, the most disruptive advancements of commercial LIBs in the past decade stem instead from overall cell design and engineering. In pursuit of higher energy density and fast-charging capability, strategies focused on tuning the properties of composite electrode architectures (e.g., porosity, conductivity, tortuosity, spatial heterogeneity) by restructuring the inactive component matrix of LIB electrode films have recently garnered attention. This perspective explores recent advances in electrode design through an applied lens, emphasizing synthetic platforms and future research directions that are scalable, commercially feasible, and applicable to a wide range of active materials. We introduce and critically assess recently proposed strategies for structuring electrode architectures, including spatial gradients of local composition and microstructure; metal-foil current collector alternatives; and electrode templating techniques, evaluating both achievements in battery performance and commercial applicability. Coupled with improved active materials, new electrode architectures hold promise to unlock next generation LIBs.

With their excellent reliability and environmental friendliness, zinc-ion batteries (ZIBs) are regarded as potential energy storage technologies. Unfortunately, their poor cycling durability and low Coulombic effectiveness (CE), driven by dendritic growth and surface passivation on the Zn anode, severely restrict their commercialization. Herein, we describe the in situ construction of a Zn-rich polymeric solid–electrolyte interface (SEI) using polyacrylic acid (PAA) as an electrolyte additive. On the one hand, the PAA SEI layer offers evenly distributed nucleation sites and promotes ion transport, hence suppressing dendrite growth. On the other hand, the SEI layer prevents direct contact between the Zn foil and the electrolyte, thus inhibiting side reactions. Additionally, the robust coordination of PAA with Zn²⁺ and the SEI layer's good adherence to the Zn foil provide long-term protection to the Zn anode. As a result, symmetric cells and Zn/V₂O₅ cells all deliver prolonged cycle life and superior electrochemical efficiency.

Lithium metal batteries are regarded as promising alternative next-generation energy storage systems. However, the unstable anode interphase results in dendrite growth and irreversible lithium consumption with low Coulombic efficiency (CE). Herein, we rationally design a Li⁺ coordination structure via electrolyte solvation chemistry. Nitrate anions are aggregated in the solvation sheath, even at low concentration in a solvent with moderate solvation ability, which promotes Li⁺ desolvation and constructs a nitrate anion-tuned interphase. Meanwhile, a high-donor-number solvent is introduced as an additive to strongly coordinate with Li⁺, which accelerates the ion-transfer kinetics and rate performance. This not only results in micro-sized lithium deposition and a high CE of 99.5% over 3500 ​h, but also enables superior anode stability even under 50% depth plating/stripping and with a lean electrolyte of 3 ​g ​Ah⁻¹ at 50 ​°C. A lithium–sulfur battery exhibits a prolonged lifespan of 2000 cycles with an average CE of 100%. A full battery using 1x excess lithium exhibits a high capacity near 1600 ​mAh ​g_S⁻¹ for 100 cycles without capacity loss. Moreover, a 0.55 ​Ah pouch cell delivers a reversible energy density of 423 ​Wh ​kg⁻¹ based on these electrodes and electrolyte.

Electrochemical CO₂ reduction is a typical surface-mediated reaction, with its reaction kinetics and product distributions largely dependent on the dynamic evolution of reactive species at the cathode–catholyte interface and on the resultant mass transport within the hydrodynamic boundary layer in the vicinity of the cathode. To resolve the complex local reaction environment of branching CO₂ reduction pathways, we here present a differential electrochemical mass spectroscopic (DEMS) approach for Cu electrodes to investigate CO₂ mass transport, the local concentration gradients of buffering anions, and the Cu surface topology effects on CO₂ electrolysis selectivity at a temporal resolution of ∼400 ​ms. As a proof of concept, these tuning knobs were validated on an anion exchange membrane electrolyzer, which delivered a Faradaic efficiency of up to 40.4% and a partial current density of 121 ​mA ​cm⁻² for CO₂-to-C₂H₄ valorization. This methodology, which bridges the study of fundamental surface electrochemistry and the upgrading of practical electrolyzer performance, could be of general interest in helping to achieve a sustainable circular carbon economy.

Achieving carbon neutrality is an essential part of responding to climate change caused by the deforestation and over-exploitation of natural resources that have accompanied the development of human society. The carbon dioxide reduction reaction (CO₂RR) is a promising strategy to capture and convert carbon dioxide (CO₂) into value-added chemical products. However, the traditional trial-and-error method makes it expensive and time-consuming to understand the deeper mechanism behind the reaction, discover novel catalysts with superior performance and lower cost, and determine optimal support structures and electrolytes for the CO₂RR. Emerging machine learning (ML) techniques provide an opportunity to integrate material science and artificial intelligence, which would enable chemists to extract the implicit knowledge behind data, be guided by the insights thereby gained, and be freed from performing repetitive experiments. In this perspective article, we focus on recent advancements in ML-participated CO₂RR applications. After a brief introduction to ML techniques and the CO₂RR, we first focus on ML-accelerated property prediction for potential CO₂RR catalysts. Then we explore ML-aided prediction of catalytic activity and selectivity. This is followed by a discussion about ML-guided catalyst and electrode design. Next, the potential application of ML-assisted experimental synthesis for the CO₂RR is discussed. Finally, we present specific challenges and opportunities, with the aim of better understanding research and advancements in using ML for the CO₂RR.

Adsorbent-assisted air water harvesting (AWH) may help alleviate the current global freshwater scarcity crisis. However, the weak sorption capacity of various adsorbents and the high energy required to release water are two long-standing problems. Herein, we propose a class of green and clean adsorbent, TpPa-1@LiCl composite, whose sorption capacity is greatly improved to 0.37 and 0.80 ​g ​g⁻¹ under 30% and 90% relative humidity (RH), respectively, and which has excellent stability, showing only a slight decrease (0.79%) after 10 sorption–desorption cycles (1400 ​min). This TpPa-1@LiCl composite can reach equilibrium within 2 ​h and undergo complete desorption in 30 ​min under air mass 1.5 ​G irradiation. A corresponding solar-driven AWH device can complete up to 4 sorption–desorption cycles per day, with each cycle capable of collecting 0.34 ​g ​g⁻¹ water without additional energy input, which implies TpPa-1@LiCl composite has the potential for achieving sorption-assisted AWH with high efficiency and rapid cycling.

Lithium–oxygen (Li–O₂) batteries have great potential for applications in electric devices and vehicles due to their high theoretical energy density of 3500 ​Wh kg⁻¹. Unfortunately, their practical use is seriously limited by the sluggish decomposition of insulating Li₂O₂, leading to high OER overpotentials and the decomposition of cathodes and electrolytes. Cathode electrocatalysts with high oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) activities are critical to alleviate high charge overpotentials and promote cycling stability in Li–O₂ batteries. However, constructing catalysts for high OER performance and energy efficiency is always challenging. In this mini-review, we first outline the employment of advanced electrocatalysts such as carbon materials, noble and non-noble metals, and metal–organic frameworks to improve battery performance. We then detail the ORR and OER mechanisms of photo-assisted electrocatalysts and single-atom catalysts for superior Li–O₂ battery performance. Finally, we offer perspectives on future development directions for cathode electrocatalysts that will boost the OER kinetics.