Semiconductor-based materials utilized in photocatalysts and electrocatalysts present a sophisticated solution for efficient solar energy utilization and bias control, a field extensively explored for its potential in sustainable energy and environmental management. Recently, 3D printing has emerged as a transformative technology, offering rapid, cost-efficient, and highly customizable approaches to designing photocatalysts and electrocatalysts with precise structural control and tailored substrates. The adaptability and precision of printing facilitate seamless integration, loading, and blending of diverse photo(electro)catalytic materials during the printing process, significantly reducing material loss compared to traditional methods. Despite the evident advantages of 3D printing, a comprehensive compendium delineating its application in the realm of photocatalysis and electrocatalysis is conspicuously absent. This paper initiates by delving into the fundamental principles and mechanisms underpinning photocatalysts electrocatalysts and 3D printing. Subsequently, an exhaustive overview of the latest 3D printing techniques, underscoring their pivotal role in shaping the landscape of photocatalysts and electrocatalysts for energy and environmental applications. Furthermore, the paper examines various methodologies for seamlessly incorporating catalysts into 3D printed substrates, elucidating the consequential effects of catalyst deposition on catalytic properties. Finally, the paper thoroughly discusses the challenges that necessitate focused attention and resolution for future advancements in this domain.

Additive Manufacturing: A Paradigm Shift in Revolutionizing Catalysis with 3D Printed Photocatalysts and Electrocatalysts Toward Environmental Sustainability.

Antibiotic residues in aquatic environments can be effectively degraded by hydroxyl radical (OH)-based advanced oxidation processes (AOPs). However, the reaction kinetics and mechanisms have not been comprehensive determined due to the limitations of conventional competition kinetic methods and mass spectrometry-based product identification, as these methods fail to exclude interference from secondary radicals and are unable to capture unstable intermediates or transient species. In this study, these limitations were overcome using laser flash photolysis (LFP) and density functional theory (DFT) calculations, allowing accurate determination of the OH-initiated reaction kinetics and degradation mechanisms of florfenicol (FF), a model veterinary antibiotic compound that is frequently detected in the environment. Based on the LFP experiment results, the second order rate constant (k) between OH and FF was determined to be 1.96 × 109 M−1 s−1 by tracking the typical signal of (SCN)2−. Furthermore, DFT calculations revealed two distinct mechanisms for OH addition to the benzene ring and identified hydrogen atom abstraction (HAA) reaction from chiral carbons as being the most favorable initial reaction for OH. In addition, the destruction of chlorine moiety occurred via hydroxylation-chlorine abstraction, rather than direct chlorine abstraction or substitution reactions. The resistance of chlorine moiety to degradation during the initial oxidation process, resulted in the formation of chlorine-containing by-products. This study provided a novel approach to comprehensively investigate the mechanisms of emerging contaminants elimination during OH-based AOPs. 

Mechanistic and kinetic aspects of florfenicol degradation by OH: Chloride moiety resistance

Compared with conventional wastewater treatment processes, electrochemical oxidation processes (EOPs) can remove hazardous substances from wastewater more efficiently and without pollution. With the rapid development of green power technology, there are more development prospects for EOPs in wastewater treatment. In recent years, research related to EOPs in the field of wastewater treatment has flourished, numerous researchers have reviewed the last advances. However, the key challenges and future directions of EOPs in the context of carbon neutrality are still under-analyzed. In this review, we first summarize the oxidation mechanism and various control factors of EOPs. Then, we discuss the current development status of current and emerging electrode materials, and summarize their commonly used evaluation criteria and systems. Finally, based on the above review, we analyze the key challenges faced by EOPs in theoretical research and practical applications, and propose potential directions for the development of EOPs in wastewater treatment to meet the growing demand for carbon neutrality. We believe that this review will offer crucial guidance and reference to enhance the application and dissemination of EOPs in organic wastewater treatment. 

Electrochemical oxidation processes based on renewable energy towards carbon neutrality: Oxidation fundamentals, catalysts, challenges and prospects

The three-dimensional electrode (3DE) process has attracted much attention due to its high efficiency in treating hard-to-degrade organic pollutants. In this work, an efficient removal of low-concentration tetracycline (TC) from aqueous solution was achieved using a 3DE reactor equipped with IrO2-RuO2-Ti anode and granular activated carbon (GAC). In addition, the reliable response surface model (RSM) indicates that maintaining a current density of 12.5 mA/cm2 led to effective TC degradation (≥ 96%) within two hours. After verification, •OH and •O2− were identified as the primary active oxygen species in the 3DE system and the addition of particle electrodes significantly enhanced the system's ability to generate •O2−. Additionally, we proposed the complete degradation pathway for TC in the 3DE system, utilizing LC-MS and DFT calculations. Notably, the 3DE system demonstrates superior detoxification efficiency. Many highly toxic intermediates detoxify into minimal amounts of less toxic substances after degradation and exhibit a growth-promoting ability for mung beans comparable to that of pure water. Meanwhile, the outstanding universality, stability, and cost-effectiveness of 3DE systems also contribute to its extensive application prospects. The study presents an efficient, cost-effective, and viable process scheme for removing low-concentration TC from aqueous solutions. 

Electrochemical oxidation of low concentrated tetracycline (TC) in aqueous solution: Operation optimization, degradation mechanisms, and detoxification efficiency

Cu/Mn-mediated electron shuttle and high-valent metals enhance hydroxyl radicals production during the electrochemical oxidation on the CuMn-Sb-SnO2 electrode

In this study, a novel 3D printed (3DP) Nb2O5/Ti electrode with a three-dimensional pore structure was prepared using selective laser melting (SLM) 3DP technology. The electrode exhibited high degradation efficiency, low energy consumption (16.02 Wh/L for 90% removal of 5 mg/L of Florfenicol (FLO)), and promising lifetime. Specifically, the 3DP 3% Nb2O5/Ti electrode maintained a 97.0% degradation efficiency for FLO within 120 min when consecutively used for 20 cycles. It was proposed that the Nb2O5 served as an n-type dopant for Ti (IV), creating an electronegative surface environment that leads to stronger binding of electrons from H2O or FLO to the electrode surface. Consequently, the 3D-printed Nb2O5/Ti electrode exhibits higher OER potential and a greater yield of reactive oxygen species (ROSs) compared to the undoped Ti electrode. The electrode also achieved an 82.5% defluorination ratio for FLO, which is the best dehalogenation yield reported so far. Additionally, the toxicity of intermediates was significantly reduced after electrooxidation treatment, and 11 degradation products were identified by UPLC-MS/MS for potential degradation pathways identification. This study suggests that the 3D printed Nb2O5/Ti electrode holds great promise in remediating pharmaceuticals and personal care products (PPCPs)-contaminated water, and that SLM 3D printing technology is a beneficial method for producing Ti-stabilized anodes. 

Advanced electrooxidation of florfenicol using 3D printed Nb2O5/Ti electrodes: Degradation efficiency, dehalogenation performance, and toxicity reduction

Hydroxylate Black-Phosphorus Promote the Supercapacitive Performances of Polyaniline by 200%: From Theoretical Prediction to Prototype Device

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Advanced electrooxidation of florfenicol using 3D printed Nb2O5/Ti electrodes: Degradation efficiency, dehalogenation performance, and toxicity reduction

Hydroxylate Black-Phosphorus Promote the Supercapacitive Performances of Polyaniline by 200%: From Theoretical Prediction to Prototype Device