Semiconductor photocatalytic technology holds immense promise for converting sustainable solar energy into chemically storable energy, with significant applications in the realms of energy and the environment. However, the inherent issue of rapid recombination of photogenerated electrons and holes hinders the performance of single photocatalysts. To overcome this challenge, the construction of two-dimensional (2D) S-scheme heterojunction photocatalysts has emerged as an effective strategy. The deliberate design of dimensionality ensures a substantial interfacial area, while the S-scheme charge transfer mechanism facilitates efficient charge separation and maximizes redox capabilities. This review commences with a fresh perspective on the charge transfer mechanism in S-scheme heterojunctions, followed by a comprehensive exploration of preparation methods and characterization techniques. Subsequently, the recent advancements in 2D S-scheme heterojunction photocatalysts are summarized. Notably, the mechanism behind activity enhancement is elucidated. Finally, the prospects for the development of 2D S-scheme photocatalysts are presented. This article is protected by copyright. All rights reserved.

Construction of Two-Dimensional S-scheme Heterojunction Photocatalyst.

Present photocatalysts for the synchronous cleanup of pharmaceuticals and heavy metals have several drawbacks, including inadequate reactive sites, inefficient electron–hole disassociation, and insufficient oxidation and reduction power. In this research, we sought to address these issues by using a facile solvothermal-photoreduction route to develop an innovative plasmonic S-scheme heterojunction, Au/MIL-101(Fe)/BiOBr. The screened-out Au/MIL-101(Fe)/BiOBr (AMB-2) works in a durable and high-performance manner for both Cr(VI) and norfloxacin (NOR) eradication under visible light, manifesting up to 53.3 and 2 times greater Cr(VI) and NOR abatement rates, respectively, than BiOBr. Remarkably, AMB-2’s ability to remove Cr(VI) in a Cr(VI)-NOR co-existence system is appreciably better than in a sole-Cr(VI) environment; the synergy among Cr(VI), NOR, and AMB-2 results in the better utilization of photo-induced carriers, yielding a desirable capacity for decontaminating Cr(VI) and NOR synchronously. The integration of MOF-based S-scheme heterojunctions and a plasmonic effect contributes to markedly reinforced photocatalytic ability by increasing the number of active sites, augmenting the visible-light absorbance, boosting the efficient disassociation and redistribution of powerful photo-carriers, and elevating the generation of reactive substances. We provide details of the photocatalytic mechanism, NOR decomposition process, and bio-toxicity of the intermediates. This synergistic strategy of modifying S-scheme heterojunctions with a noble metal opens new horizons for devising excellent MOF-based photosystems with a plasmonic effect for environment purification. 

A plasmonic S-scheme Au/MIL-101(Fe)/BiOBr photocatalyst for efficient synchronous decontamination of Cr(VI) and norfloxacin antibiotic

To utilize intermittent renewable energy as well as achieve the goals of peak carbon dioxide emissions and carbon neutrality, various electrocatalytic devices have been developed. However, the electrocatalytic reactions, e.g., hydrogen evolution reaction/oxygen evolution reaction in overall water splitting, polysulfide conversion in lithium–sulfur batteries, formation/decomposition of lithium peroxide in lithium–oxygen batteries, and nitrate reduction reaction to degrade sewage, suffer from sluggish kinetics caused by multielectron transfer processes. Owing to the merits of accelerated charge transport, optimized adsorption/desorption of intermediates, raised conductivity, regulation of the reaction microenvironment, as well as ease to combine with geometric characteristics, the built-in electric field (BIEF) is expected to overcome the above problems. Here, we give a Review about the very recent progress of BIEF for efficient energy electrocatalysis. First, the construction strategies and the characterization methods (qualitative and quantitative analysis) of BIEF are summarized. Then, the up-to-date overviews of BIEF engineering in electrocatalysis, with attention on the electron structure optimization and reaction microenvironment modulation, are analyzed and discussed in detail. In the end, the challenges and perspectives of BIEF engineering are proposed. This Review gives a deep understanding on the design of electrocatalysts with BIEF for next-generation energy storage and electrocatalytic devices. 

Designing a Built-In Electric Field for Efficient Energy Electrocatalysis

Understanding charge transfer dynamics and carrier separation pathway is challenging due to the lack of appropriate characterization strategies. In this work, a crystalline triazine/heptazine carbon nitride homojunction is selected as a model system to demonstrate the interfacial electron-transfer mechanism. Surface bimetallic cocatalysts are used as sensitive probes during in situ photoemission for tracing the S-scheme transfer of interfacial photogenerated electrons from triazine phase to the heptazine phase. Variation of the sample surface potential under light on/off confirms dynamic S-scheme charge transfer. Further theoretical calculations demonstrate an interesting reversal of interfacial electron-transfer path under light/dark conditions, which also supports the experimental evidence of S-scheme transport. Benefiting from the unique merit of S-scheme electron transfer, homojunction shows significantly enhanced activity for CO2 photoreduction. Our work thus provides a strategy to probe dynamic electron transfer mechanisms and to design delicate material structures towards efficient CO2 photoreduction. 

/pdf/understanding-the-unique-s-scheme-charge-migration-in-f9gtooa2.pdf

Understanding the unique S-scheme charge migration in triazine/heptazine crystalline carbon nitride homojunction

Recent years have witnessed an upsurge of interest in exploiting advanced photo‐/electrocatalysts for efficient energy conversion and environmental remediation. Constructing internal electric fields has been highlighted as a rising star to help facilitate various catalytic processes, with the merits of promoting charge transfer/separation, optimizing redox potential and creating effective active/adsorption sites. Internal electric fields are usually formed by the polarization of uneven charge distributions between different constituent layers, which widely exist in piezoelectrics, polar surface terminations, and heterostructure materials. Herein, a groundbreaking and interdisciplinary overview of the latest advances in the construction of internal electric fields to improve photo(electro)catalytic and electrocatalytic activity is provided. This critical review begins with an encyclopedic summary of the classification, advantages, and synthesis strategies of internal electric fields. Subsequently, the identification methods are thoroughly discussed based on the characterization techniques, experiments, and theoretical calculations, which can provide profound guidance for the in‐depth study of internal electric fields. To elaborate the theory–structure–activity relationships for internal electric fields, the corresponding reaction mechanisms, modification strategies, and catalytic performance are jointly discussed, along with a discussion of their practical energy and environmental applications. Finally, an insightful analysis of the challenges and future prospects for internal electric field‐based catalysts are discussed.

Enabling Internal Electric Fields to Enhance Energy and Environmental Catalysis

Construction of internal electric fields (IEFs) is crucial to realize efficient charge separation for charge-induced redox reactions, such as water splitting and CO2 reduction. However, a quantitative understanding of the charge transfer dynamics modulated by IEFs remains elusive. Here, electron microscopy study unveils that the non-equilibrium photo-excited electrons are collectively steered by two contiguous IEFs within binary (001)/(200) facet junctions of BiOBr platelets, and they exhibit characteristic Gaussian distribution profiles on reduction facets by using metal co-catalysts as probes. An analytical model justifies the Gaussian curve and allows us to measure the diffusion length and drift distance of electrons. The charge separation efficiency, as well as photocatalytic performances, are maximized when the platelet size is about twice the drift distance, either by tailoring particle dimensions or tuning IEF-dependent drift distances. The work offers great flexibility for precisely constructing high-performance particulate photocatalysts by understanding charge transfer dynamics. 

/pdf/unveiling-the-charge-transfer-dynamics-steered-by-built-in-iqcmg3bk.pdf

Unveiling the charge transfer dynamics steered by built-in electric fields in BiOBr photocatalysts

For persulfate-based advanced oxidation process, the non-radical pathway is an important route due to the selective oxidation of pollutants and its strong tolerance to complex water bodies. However, the selective oxidation mechanism of organic pollutants needs further elaboration. Herein, we demonstrate a facile hydrothermal pretreatment and high-temperature carbonization route to synthesize the nitrogen-doped porous biochar (NHBC-1). Owing to the well-developed hierarchical porous structure, the created internal active defects, and tailored nitrogen dopants, the NHBC-1 catalyst exhibited excellent catalytic activity for peroxydisulfate (PDS) activation. The results show that pyridinic N facilitated the adsorption of PDS on NHBC-1 to form the highly active NHBC-PDS* complex. Meanwhile, graphitic N and the defective structures promoted the electron-transfer process, thus allowing the efficient catalytic performance of the NHBC/PDS system for phenol oxidation via an electron-transfer dominated pathway. In addition, the system exhibited versatile applicability for the remediation of various organic pollutants in different actual water matrices with wide pH adaptability and satisfactory mineralization efficiency. More importantly, the selective oxidation mechanism of organic contaminants was revealed. Specifically, only the pollutant with oxidation potential lower than that of the NHBC-PDS* complex (0.91 V) can be effectively eliminated. This study not only provides a facile route for the rational designing of a cost-affordable biochar catalyst for PDS activation, but also offers valuable insights into the understanding of selective oxidation of organic contaminants via an electron-transfer dominated pathway. 

Electron-transfer based selective oxidation of organic pollutants via N-doped biochar activated peroxydisulfate: Important role of oxidation potential

Interface functional groups protected by confinement effect for flexible supercapacitor and capacitive deionization

Two-dimensional polymerized carbon nitride coupled with (001)-facets-exposed titanium dioxide S-scheme heterojunction for photocatalytic degradation of norfloxacin

Effect of KBr on electrodeposition of Ag in choline chloride-ethylene glycol deep eutectic solvents

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