Perovskite solar cells(PSCs)have exhibited impressive performance,achieving a power conversion efficiency(PCE)of 26.1%.However,the water-soluble and toxic nature of lead(Pb)in PSCs hinders their industrialization.Pb chemisorption has emerged as a promising approach to address this issue to prevent Pb leakage and ensure long-term stability.This perspective provides a comprehensive overview of recent advancements in Pb chemisorption in PSCs and discusses the prospects for future developments and challenges in this field.
Metal tellurides(MTes) are highly attractive as promising anodes for high-performance potassium-ion batteries. The capacity attenuation of most reported MTe anodes is attributed to their poor electrical conductivity and large volume variation. The evolution mechanisms, dissolution properties, and corresponding manipulation strategies of intermediates(K-polytellurides, K-pTe_(x)) are rarely mentioned. Herein,we propose a novel structural engineering strategy to confine ultrafine CoTe_(2) nanodots in hierarchical nanogrid-in-nanofiber carbon substrates(CoTe_(2)@NC@NSPCNFs) for smooth immobilization of K-pTe_(x) and highly reversible conversion of CoTe_(2) by manipulating the intense electrochemical reaction process. Various in situ/ex situ techniques and density functional theory calculations have been performed to clarify the formation, transformation, and dissolution of K-pTe_(x)(K_(5)Te_(3) and K_(2)Te), as well as verifying the robust physical barrier and the strong chemisorption of K_(5)Te_(3) and K_(2)Te on S, N co-doped dual-type carbon substrates. Additionally, the hierarchical nanogrid-in-nanofiber nanostructure increases the chemical anchoring sites for K-pTe_(x), provides sufficient volume buffer space, and constructs highly interconnected conductive microcircuits, further propelling the battery reaction to new heights(3500 cycles at 2.0 A g^(-1)). Furthermore, the full cells further demonstrate the potential for practical applications. This work provides new insights into manipulating K-pTe_(x) in the design of ultralong-cycling MTe anodes for advanced PIBs.
Solid chemisorption technologies for hydrogen storage,especially high-efficiency hydrogen storage of fuel cells in near ambient temperature zone defined from−20 to 100℃,have a great application potential for realizing the global goal of carbon dioxide emission reduction and vision of carbon neutrality.However,there are several challenges to be solved at near ambient temperature,i.e.,unclear hydrogen storage mechanism,low sorption capacity,poor sorption kinetics,and complicated synthetic procedures.In this review,the characteristics and modification methods of chemisorption hydrogen storage materials at near ambient temperature are discussed.The interaction between hydrogen and materials is analyzed,including the microscopic,thermodynamic,and mechanical properties.Based on the classification of hydrogen storage metals,the operation temperature zone and temperature shifting methods are discussed.A series of modification and reprocessing methods are summarized,including preparation,synthesis,simulation,and experimental analysis.Finally,perspectives on advanced solid chemisorption materials promising for efficient and scalable hydrogen storage systems are provided.
Nitrogen chemisorption is a prerequisite for efficient ammonia synthesis under ambient conditions,but promoting this process remains a significant challenge.Here,by loading yttrium clusters onto a single-atom support,an electronic promoting effect is triggered to successfully eliminate the nitrogen chemisorption barrier and achieve highly efficient ammonia synthesis.Density functional theory calculations reveal that yttrium clusters with abundant electron orbitals can provide considerable electrons and greatly promote electron backdonation to the N2 antibonding orbitals,making the chemisorption process exothermic.Moreover,according to the“hot atom”mechanism,the energy released during exothermic N2 chemisorption would benefit subsequent N2 cleavage and hydrogenation,thereby dramatically reducing the energy barrier of the overall process.As expected,the proof-of-concept catalyst achieves a prominent NH3 yield rate of 48.1μg·h^(−1)·mg^(−1)at−0.2 V versus the reversible hydrogen electrode,with a Faradaic efficiency of up to 69.7%.This strategy overcomes one of the most serious obstacles for electrochemical ammonia synthesis,and provides a promising method for the development of catalysts with high catalytic activity and selectivity.
Yuzhuo JiangMengfan WangSisi LiuLifang ZhangSiyi QianYufeng CaoYu ChengTao QianChenglin Yan
The chemisorption energy is an integral aspect of surface chemistry,central to numerous fields such as catalysis,corrosion,and nanotechnology.Electronic-structure-based methods such as the Newns-Anderson model are therefore of great importance in guiding the engineering of material surfaces with optimal properties.However,existing methods are inadequate for interpreting complex,multi-metallic systems.Herein,we introduce a physics-based chemisorption model for alloyed transition metal surfaces employing primarily metal d-band properties that accounts for perturbations in both the substrate and adsorbate electronic states upon interaction.Importantly,we show that adsorbate-induced changes in the adsorption site interact with its chemical environment leading to a second-order response in chemisorption energy with the d-filling of the neighboring atoms.We demonstrate the robustness of the model on a wide range of transition metal alloys with O,N,CH,and Li adsorbates yielding a mean absolute error of 0.13 eV versus density functional theory reference chemisorption energies.