Ying Wang

The Scholl reaction is a cornerstone method for constructing polycyclic aromatic hydrocarbons, yet its mechanism remains highly debated because arenium and radical cation intermediates are difficult to characterize. Herein, we demonstrate that electrochemical oxidation provides precise mechanistic control: a low‐potential acidic (LPA) condition selectively favors the arenium cation pathway, whereas a high‐potential neutral (HPN) condition promotes the radical cation pathway. While it is often assumed that only one mechanism operates under a given set of chemical oxidation conditions, our results reveal that most substrates can react via both pathways. Dialkoxyphenyl groups are found to facilitate the radical cation pathway, although no general correlation with overall substrate electron richness is observed. This electrochemical control provides the experimental basis to re‐evaluate previously proposed mechanisms for certain substrates. We demonstrate that switching between LPA and HPN conditions yields different products from the same 3,3’‐diphenyl‐2,2′‐binaphthalene substrate, thereby correcting the computational assignment of the corresponding pathways. Additionally, we show that a tetracene‐derived substrate undergoes cyclodehydrogenation through the arenium cation pathway, revising the computationally assigned dication mechanism for this transformation. Collectively, these results establish electrochemistry as a powerful alternative to traditional chemical oxidation, offering unprecedented experimental control to resolve fundamental mechanistic debates about the Scholl reaction.

The Scholl reaction is a cornerstone method for constructing polycyclic aromatic hydrocarbons, yet its mechanism remains highly debated because arenium and radical cation intermediates are difficult to characterize. Herein, we demonstrate that electrochemical oxidation provides precise mechanistic control: a low‐potential acidic (LPA) condition selectively favors the arenium cation pathway, whereas a high‐potential neutral (HPN) condition promotes the radical cation pathway. While it is often assumed that only one mechanism operates under a given set of chemical oxidation conditions, our results reveal that most substrates can react via both pathways. Dialkoxyphenyl groups are found to facilitate the radical cation pathway, although no general correlation with overall substrate electron richness is observed. This electrochemical control provides the experimental basis to re‐evaluate previously proposed mechanisms for certain substrates. We demonstrate that switching between LPA and HPN conditions yields different products from the same 3,3’‐diphenyl‐2,2′‐binaphthalene substrate, thereby correcting the computational assignment of the corresponding pathways. Additionally, we show that a tetracene‐derived substrate undergoes cyclodehydrogenation through the arenium cation pathway, revising the computationally assigned dication mechanism for this transformation. Collectively, these results establish electrochemistry as a powerful alternative to traditional chemical oxidation, offering unprecedented experimental control to resolve fundamental mechanistic debates about the Scholl reaction.

This review highlights recent progress in low-concentration CO ₂ electrochemical capture and conversion via capture–conversion coupling and direct dilute CO ₂ electrolysis, focusing on catalyst design and electrolyzer engineering.

Metal‐support interactions provide a powerful tool to tailor the catalytic activities of metallic catalysts. Amorphous materials can serve as an effective support matrix to form unique crystalline‐amorphous interfaces and modulate the electronic structure of active metals. However, robust synthetic strategies for precise structural control remain underdeveloped. Here, we report the laser‐shocked synthesis of heterostructures including bimetallic CuNi, CuFe, CuCo, and medium‐entropy CuFeCoNi heterostructures, where crystalline metal nanoparticles are anchored on amorphous hydroxide supports. The heterostructures are characterized by an interfacial electronic distribution that improves catalytic activities. With CuNi as an example for nitrate reduction reaction, the laser‐engineered heterophase CuNi achieves an NH ₃ production rate of 92.18 mg/h/mg _cat with 98.6% Faradaic efficiency (FE), substantially superior to standalone crystalline CuNi or amorphous CuNi hydroxide. The CuNi heterostructure maintains a stable FE(NH ₃ ) of ∼90% up to 80 h while improving current density from 75 to 120 mA/cm ² due to the robust amorphous layer and dynamic amorphous/crystalline reconstruction. In situ characterization and theoretical calculations reveal that the amorphous/crystalline interface regulates the balance between reactive hydrogen species and reaction intermediates, effectively suppressing the competing hydrogen evolution and promoting cascade nitrate‐to‐nitrite and nitrite‐to ammonia conversion. This work provides a general and viable strategy for producing high‐performance supported catalysts.

Aqueous redox flow batteries are promising for long-duration energy storage. However, many of them (e.g. sulfur-based and organic-based flow batteries) suffer from sluggish kinetics with low energy efficiency and insufficient capacity utilization. Here, we propose relay catalysis as a universal strategy to achieve high reaction rates while minimizing overpotential, enabling high capacity and energy efficiency. Inspired by sequential electron transfer in cellular respiration, relay catalysis employs a low-overpotential catalyst (e.g., isoalloxazine) to initiate the reaction, seamlessly transferring control to a high-activity catalyst (e.g., quinone) to sustain charge propagation, breaking the trade-off between overpotential and catalytic rate. Using this strategy, we demonstrate polysulfide-ferrocyanide flow batteries with near full polysulfide utilization (S ₄ ^2– /S ₂ ^2– , 64 Ah L ^–1 _negolyte ) and high stability over 3 months (> 500 cycles at 20 mA cm ^–2 , decay rate 0.00071% per cycle, 0.003% per day). We further extend this strategy to organosulfide- and azo-based batteries with various relay-catalyst couples. By mimicking biological electron relays, this approach not only redefines homogeneous catalysis for energy storage but also establishes a transformative platform for designing flow batteries with enhanced performance and scalability.

This review summarizes the progress of catalyst design and reactor optimization in non-thermal plasma for converting CO ₂ and CH ₄ into value-added oxygenates.

Temperature is a critical parameter that can significantly influence the outcome of the redox reactions. However, determining the temperature-dependent properties of redox couples is often time-consuming and susceptible to inconsistencies. In this work, we present a temperature-controlled electrochemical station capable of acquiring electrochemical measurements under preprogrammed conditions to extract key thermodynamic parameters. We demonstrate the functionality of this system using electrochemical impedance spectroscopy to determine the activation energies of the [Fe­(CN)₆]^3–/^4– redox couple and the hydrogen evolution reaction on platinum and gold electrodes. Additionally, we illustrate automated cyclic voltammetry data acquisition for [Fe­(CN)₆]^3–/^4–, [Ru­(NH₃)₆]²⁺/³⁺, benzoquinone, and anthraquinone. By analyzing the temperature-dependent shifts in E _1/2, we calculated the entropy changes and thermogalvanic coefficients of these systems. Furthermore, we examined the entropy variations of ferricyanide in mixed aqueous–organic electrolytes, highlighting the role of solvation reconfiguration. The versatility of this setup offers a robust and efficient platform for the rapid characterization of temperature-dependent redox properties, with implications for energy conversion and sensing applications.