Carbon Neutralization最新文献

Front cover image: The cover image presents a Sr-substituted two-dimensional (2D) porous LaFeO₃ perovskite catalyst for electrocatalytic oxygen evolution applications. In article number 10.1002/cnl2.94, Wan and Jin et al. demonstrate a microwave shock strategy to realize a synergistic combination of electronic configuration and 2D structural design for unveiling the structure-activity relationship in 2D perovskite electrocatalysts.

Inside back cover image: The effective storage and utilization of hydrogen energy is expected to solve the problems of energy shortage and environmental pollution currently faced by human society. To solve the problems of directional design and rational construction of new MOFs, in article number 10.1002/cnl2.91, the authors use the principles and methods of coordination chemistry and crystal engineering to carry out the theoretical design and mechanism research of new MOFs for high-efficiency hydrogen storage application scenarios.

In recent years, the development of photocatalysts based on noncovalent strategies has shown an important role in medical and organic materials. Herein, an organic fluorescent dye benzothiazole derivative (2-(N,N-diethylanilin-4-yl)-4,6-bis(3-methylpyrazol-1-yl)-1,3,5-triazine [MPBT]) was designed and synthesized. It was encapsulated in the cavity of cucurbit[8]uril (CB[8]) to form a supramolecular dimer through host–guest interaction, which converted the dye into a highly efficient photocatalyst. With the formation of 2MPBT-CB[8] supramolecular dimer, the emergence of host-enhanced charge transfer interactions could significantly facilitate singlet to triplet through intersystem crossing. At the same time, the alternating structure of 2MPBT-CB[8] facilitated the triplet states for further energy transfer and electron transfer. In addition, the electron transfer process with electron donor generated cationic free radical and photocatalyst negative ion free radical (), which in turn reacted with oxygen (O₂) to form superoxide anion radical (). The generated could be used to catalyze the oxidative hydroxylation of aryl boronic acid. Therefore, the 2MPBT-CB[8] had become a highly efficient photocatalyst for the oxidative hydroxylation of aryl boronic acid. This strategy of supramolecular dimerization provides a new strategy for the development of new photocatalysts based on noncovalent interactions.

Hybrid supercapacitors (HSCs) comprising a battery-type cathode and capacitive anode have recently become a research hotspot. Nevertheless, the low capacity utilization, poor kinetic behavior, and unstable structure of a single battery-type oxide cathode restrict the overall performance of the device. Herein, the carbon quantum dots (CQDs) modified NiO/Co₃O₄ heterostructured flower-like microspheres are constructed, and enhanced specific capacity, rate capability, and cycling performance are achieved when used as the cathode for HSCs. This is attributed to the fact that the modification of bifunctional CQDs as size regulators and conductive agents and the construction of heterostructure can not only improve the specific surface area and provide more electroactive sites, thereby enhancing the charge storage performance but also regulate the electronic structure and boost the interface charge transfer capability and electronic conductivity, thereby boosting the reaction kinetics and cycle stability. The enhanced electrochemical kinetic behavior is revealed by electrochemical kinetic analyses based on cyclic voltammetry, electrochemical impedance spectroscopy tests and density functional theory calculations. Meanwhile, the electrochemical reaction process and energy storage mechanism are illustrated by ex-situ X-ray diffraction and X-ray photoelectron spectroscopy characterizations. Furthermore, an HSC is further constructed using the CQDs/NiO/Co₃O₄ heterostructured flower-like microspheres as the cathode, simultaneously achieving high energy density (40.9 Wh kg⁻¹), high power density (24 kW kg⁻¹), and splendid cyclic stability (94.2% capacity retention after 5000 cycles at 10 A g⁻¹). These synergistic modification strategies of bifunctional CQDs modification and heterostructure design provide a valuable direction for the design and development of HSCs with both high energy density and high power density.

Due to γ-Bi₂MoO₆ (BMO) has attracted considerable attention because of its unique layered perovskite structure and excellent electrical conductivity. However, the easy recombination of electron–hole pairs limits its practical application. To address this issue, we successfully prepared aliovalent Cd²⁺ doped BMO (Cd-BMO) by using a simple hydrothermal method for the degradation of the sulfamethoxazole (SMZ) and Rhodamine B (RhB). The result found that the degradation efficiency of Cd-BMO is significantly higher than that of BMO, despite an increase in the bandgap after the introduction of Cd²⁺. The superior degradation efficiency of 8% Cd-BMO, with a smaller particle size and larger specific surface area, can be attributed to its fast charge separation efficiency, low charge transfer resistance, and low rate of electron–hole pair recombination. Repeated and ion spillover experiments prove that 8% Cd-BMO shows good stability and environmental protection. Theoretical simulation demonstrates that Cd offers electrons to the BMO system due to the decreased binding energy of BMO. The 8% Cd-BMO sample can provide a suitable electric band edge for generating dominant active radicals during degradation. This work not only provides a potential candidate of 8% Cd-BMO for practical degradation but also sheds light on the design of superior photocatalysts.

The development of organic lithium batteries (OLBs) offers a promising opportunity for the advancement of green and sustainable energy storage systems. However, organic cathode materials face challenges in terms of conductivity, electrochemical activity, and dissolution. Here, we address these limitations by introducing a sulfur-linked carbonyl compound called poly(dichlorobenzoquinone sulfide) (PDBS), which is polymerized in situ on reduced graphene oxide by a mixed solvent thermal method. The resulting carbonyl compound electrode materials exhibit favorable properties as organic cathode materials for OLBs. After 4000 cycles at a current density of 1000 mA g⁻¹, the carbonyl compound electrodes exhibit a discharge capacity of 102 mAh g⁻¹. This remarkable performance indicates excellent stability and long cycle life, which are crucial for practical applications. These results suggest that PDBS, a designable sulfur-linked carbonyl compound, holds great promise as an effective organic cathode material for OLBs. In addition, this work provides valuable insights into improving the electrochemical performance of organic cathode materials.

Developing an efficient and stable oxygen evolution reaction (OER) catalyst is beneficial in various energy conversion and storage applications for achieving the “Carbon Neutrality” goal. Among the iron-based perovskite oxides (AFeO₃), LaFeO₃ stands out as a preferred catalyst for electrocatalytic OER due to its exceptional selectivity in oxygen bonding at the A-site. The introduction of A-site substitution and controlled morphological engineering in perovskite structures has proven effective in enhancing the electrical conductivity and intrinsic catalytic activity. Nevertheless, the conventional A-site substitution approach often involves prolonged high-temperature calcination, leading to the agglomeration of nanostructures, particularly in two-dimensional (2D) porous configurations. Herein, we introduce a novel method for synthesizing 2D porous LaFeO₃ perovskite with A-site Sr substitution using microwave shock. This microwave technique capitalizes on the benefits of transient heating and cooling, enabling simultaneous construction of 2D porous morphology and precise regulation of Sr substitution in one step. By conducting theoretical simulations of the electron configuration and analysis of crystal structure, we unveil the impact of Sr substitution on the OER activity of 2D porous LaFeO₃. The synthesized La_0.2Sr_0.8FeO₃ (LSFO-8) catalyst exhibits an exceptional overpotential of 339 mV at 10 mA cm⁻² and a small Tafel slope of 56.84 mV dec⁻¹ in alkaline electrolyte. This investigation provides a fresh perspective for the design and engineering of electronic configuration in highly active 2D perovskite materials.

The rational construction of Ti₃C₂T_x MXene-based composites has been deemed as a popular way to improve their electrochemical energy storage performances owing to the unique two-dimensional (2D) structure, excellent conductivity, and good flexibility. However, it remains a major challenge to assemble mesoporous carbon onto Ti₃C₂T_x with fewer oxygen-containing groups by using surfactants with short hydrophilic segments. In the work, we propose a molecular engineering assembly strategy for the growth of N,P co-doped mesoporous carbon onto Ti₃C₂T_x nanosheets (NPMC/Ti₃C₂T_x) under the assistance of phytic acid by using melamine-formaldehyde resin and pluronic P123 (PEO₂₀PPO₇₀PEO₂₀) as the carbon/nitrogen source and soft template, respectively. The detailed investigations reveal that phytic acid with abundant hydroxyl groups can effectively enhance the hydrogen bond interactions among P123, carbon precursor, and Ti₃C₂T_x nanosheets, thus ensuring the efficient assembly of mesoporous carbon onto Ti₃C₂T_x. The obtained NPMC/Ti₃C₂T_x composite demonstrates a set of merits, including cylindrical mesopore, N,P co-doping, and a good combination of mesoporous carbon and Ti₃C₂T_x nanosheets. As a result, it exhibits an improved lithium-ion storage performance, delivering a high reversible capacity of 556.3 mA h g⁻¹ after 100 cycles at 0.1 A g⁻¹. The present work provides a feasible molecular engineering assembly route for the rational design of high-performance Ti₃C₂T_x MXene-based electrodes.

Two-dimensional (2D) transition metal carbonitrides/nitrides (MXene) materials have proven to be promising alternatives as novel capacitor-type electrodes for aqueous Zn-ion hybrid microsupercapacitors (ZHMSCs). However, during self-assembly processes, serious restacking between 2D MXene nanosheets induced by strong van der Waals forces makes ion transport channels narrow within the compact MXene film electrodes, which would result in poor energy output of ZHMSCs. Herein, interlayer transport channel engineering is designed by intercalating bacterial cellulose (BC) between MXene interlayers to develop MXene/BC electrodes with fast ion transport channels in contrast to pure MXene electrodes. Benefiting from fast anion intercalation/deintercalation on MXene/BC capacitor-type cathode and reversible Zn stripping/plating on Zn foil anode, the fabricated ZHMSCs exhibit wide working potential windows (1.36 V), high areal capacitance (404 mF cm⁻²), and landmark areal energy density (94 µWh cm⁻² at 1 mA cm⁻²). The areal capacitance and energy density of the developed ZHMSCs are much higher than those of the ZHMSCs based on pure MXene capacitor-type cathode (239 mF cm⁻²/57 µWh cm⁻² at 1 mA cm⁻²). Besides, the developed ZHMSCs can perform more than 10,000 cycles, showing outstanding capacity retention. In general, our work provides a novel strategy to break through the performance bottlenecks afflicting MXene-based ZHMSCs.

In this study, we synthesized a novel corrosion inhibitor derived from thiophene and conducted a comprehensive evaluation of its inhibitory properties through both experimental and theoretical approaches. Our investigation encompassed experimental assessments employing Mass loss tests and electrochemical techniques. Additionally, we performed computational studies to delve into the electronic structure and bonding characteristics of the inhibitor, aiming to elucidate its inhibitory mechanism. Our findings revealed that the synthesized inhibitor displayed remarkable inhibitory efficiency, demonstrating its effectiveness in preventing the corrosion of mild steel. Specifically, the thiophene derivative exhibited an impressive inhibitory efficiency of 92.8%, underscoring its potential as a robust corrosion inhibitor for mild steel. Furthermore, this study delved into optimizing the conditions for employing the thiophene derivative as a corrosion inhibitor. Our investigation revealed that the most effective inhibition was achieved at a concentration of 0.5 mM and a temperature of 303 K. To elucidate the interaction between the inhibitor and the mild steel surface, we applied the Langmuir adsorption isotherm concept, shedding light on both the physical and chemical adsorption processes of the thiophene derivative on the metal's surface. Our investigations demonstrated that the addition of the inhibitor significantly reduced the corrosion rate of the metal. Our computational results further reinforced these experimental findings, indicating that the inhibitor formed stable adsorption complexes on the metal surface. This dual confirmation from experimental and computational approaches strengthens the confidence in the inhibitor's efficacy in mitigating corrosion.