Recently emerged Z-scheme heterostructure-based immunoassays have presented new opportunities for photoelectrochemical (PEC) biosensing development. Here, we described a tunable signal-on PEC biosensor for the detection of cardiac troponin I (cTnI), which exploited a competitive absorption effect between Cu(II) ions and a Zr metal-organic framework (Zr-MOF) constructed on TiO2 nanorods (Cu2+@Zr-MOF@TiO2 NRs). Water-stable Zr-MOF was coated onto TiO2 NRs on fluorine-doped tin oxide to form a Z-scheme heterostructure substrate (Zr-MOF@TiO2 NRs), which exhibited a high photoelectric response. Cu2+@Zr-MOF@TiO2 NRs, constructed by loading Cu(II) ions onto the architecture of Zr-MOF by electrostatic interaction, demonstrated a low background signal. After sandwich immunorecognition within a 96-well plate, H2S, generated by confined alkaline phosphatase on zeolitic imidazolate framework-8, was directed to react with Cu(II) ions to form CuS. This resulted in an in situ change in the photoelectrode and an enhanced photoelectric signal. The developed PEC biosensing platform exhibited high sensitivity and selectivity for the cTnI immunoassay with a detection limit of 8.6 pg/mL. The Z-scheme-based competition absorption modulation of photoelectrochemistry provides a new strategy for general PEC biosensing development.

Tunable Competitive Absorption-Induced Signal-On Photoelectrochemical Immunoassay for Cardiac Troponin I Based on Z-Scheme Metal-Organic Framework Heterojunctions.

A review on photo-, electro- and photoelectro- catalytic strategies for selective oxidation of alcohols

Energy from renewable resources is central to environmental sustainability. Among the renewables, sunlight-driven fuel synthesis is a sustainable and economical approach to produce vectors such as hydrogen through water splitting. The photocatalytic water splitting is limited by the water oxidation half-reaction, which is kinetically and energetically demanding and entails designer photocatalysts. Such challenges can be addressed by employing alternative oxidation half-reactions. Photoreforming can drive the breakdown of waste plastics and biomass into valuable organic products for the production of H2. We provide an overview of photoreforming and its underlying mechanisms that convert waste polymers into H2 fuels and fine chemicals. This is of paramount importance from two complementary perspectives: (i) green energy harvesting and (ii) environmental sustainability by decomposing waste polymers into valuables. Competitive results for the generation of H2 fuel without environmental hazards through photoreforming are being generated. The photoreforming process, mechanisms, and critical assessment of the field are scarce. We address such points by focusing on (i) the concept of photoreforming and up-to-date knowledge with key milestones achieved, (ii) uncovering the concepts and challenges in photoreforming, and (iii) the design of photocatalysts with underlying mechanisms and pathways through the use of different polymer wastes as substrates.

Photoreforming of Waste Polymers for Sustainable Hydrogen Fuel and Chemicals Feedstock: Waste to Energy.

Water electrolysis, driven by renewable energy resources, is a promising energy conversion technology that has gained intensive interest in recent years. However, conventional water electrolysis faces a number of challenges, including large thermodynamic potential gaps, valueless anodic products, explosive hydrogen/oxygen mixtures, reactive oxygen species, and limited pure water. Hybrid water electrolysis, appending different electrolytes in the anode compartment to circumvent the above‐mentioned challenges in conventional water electrolysis, is a particularly attractive alternative. In this review, for the first time, a holistic and subtle description of hybrid water electrolysis is provided, focusing on the design of high‐activity/selectivity/stability anodic electrocatalysts for the electrochemical oxidation of various chemicals, such as alcohol, aldehyde, amine, urea and hydrazine, or the oxygen evolution reaction in seawater electrolytes. Comprehensive judging criteria for anodic oxidation reactions, electrocatalysts, and reaction parameters in hybrid water electrolysis are discussed. Some technoeconomic assessments, feasibility analyses, mechanism explorations, and correlation comparisons are involved. Finally, perspectives on and opportunities for future research directions in hybrid water electrolysis systems are outlined.

Circumventing Challenges: Design of Anodic Electrocatalysts for Hybrid Water Electrolysis Systems

Photoelectrochemical reaction is emerging as a powerful approach for biomass conversion. However, it has been rarely explored for glucose conversion into value-added chemicals. Here we develop a photoelectrochemical approach for selective oxidation of glucose to high value-added glucaric acid by using single-atom Pt anchored on defective TiO2 nanorod arrays as photoanode. The defective structure induced by the oxygen vacancies can modulate the charge carrier dynamics and band structure, simultaneously. With optimized oxygen vacancies, the defective TiO2 photoanode shows greatly improved charge separation and significantly enhanced selectivity and yield of C6 products. By decorating single-atom Pt on the defective TiO2 photoanode, selective oxidation of glucose to glucaric acid can be achieved. In this work, defective TiO2 with single-atom Pt achieves a photocurrent density of 1.91 mA cm-2 for glucose oxidation at 0.6 V versus reversible hydrogen electrode, leading to an 84.3 % yield of glucaric acid under simulated sunlight irradiation. 

https://www.nature.com/articles/s41467-023-35875-9.pdf

Selective photoelectrochemical oxidation of glucose to glucaric acid by single atom Pt decorated defective TiO2

Photoelectrocatalytic (PEC) glycerol oxidation offers a sustainable approach to produce dihydroxyacetone (DHA) as a valuable chemical, which can find use in cosmetic, pharmaceutical industries, etc. However, it still suffers from the low selectivity (≤60%) that substantially limits the application. Here, we report the PEC oxidation of glycerol to DHA with a selectivity of 75.4% over a heterogeneous photoanode of Bi2O3 nanoparticles on TiO2 nanorod arrays (Bi2O3/TiO2). The selectivity of DHA can be maintained at ∼65% under a relatively high conversion of glycerol (∼50%). The existing p-n junction between Bi2O3 and TiO2 promotes charge transfer and thus guarantees high photocurrent density. Experimental combined with theoretical studies reveal that Bi2O3 prefers to interact with the middle hydroxyl of glycerol that facilitates the selective oxidation of glycerol to DHA. Comprehensive reaction mechanism studies suggest that the reaction follows two parallel pathways, including electrophilic OH* (major) and lattice oxygen (minor) oxidations. Finally, we designed a self-powered PEC system, achieving a DHA productivity of 1.04 mg cm-2 h-1 with >70% selectivity and a H2 productivity of 0.32 mL cm-2 h-1. This work may shed light on the potential of PEC strategy for biomass valorization toward value-added products via PEC anode surface engineering.

Selective Photoelectrocatalytic Glycerol Oxidation to Dihydroxyacetone via Enhanced Middle Hydroxyl Adsorption over a Bi2O3-Incorporated Catalyst.

Abstract Utilizing sustainable electrocatalysis to upcycle glycerol (GLY; the by‐product of biodiesel) to lactic acid (LA; the key monomers for biodegradable polymer) is an efficient way to reduce the cost of biodiesel, which is also consistent with the waste‐to‐wealth principle. However, current research still suffers from issues of low LA selectivity (&lt;80%), especially at high current density. Herein, we designed a cooperative catalyst by modifying BiO x nanolayers on gold nanoparticles (BiO x /Au), achieving high LA selectivity (82%) at high current density (226 mA cm −2 at 1.05 V vs. RHE), outperforming most of the reported works in the literature. We reveal that BiO x could promote the adsorption of the middle hydroxyl of GLY, which facilitates the formation of DHA and thus enables high LA selectivity. Moreover, the electron‐deficient Au in BiO x /Au is responsible for the enhanced current density, which is more beneficial to generate reactive oxygen species (OH*). To further reveal the application potential of this electrocatalytic strategy, we realized that the conversion of crude GLY extracted from cooking oil to LA coupled with H 2 production using a membrane‐free flow electrolyzer, demonstrating a sustainable fashion to convert biodiesel waste into high value‐added product and H 2 fuel. 

Selective electrooxidation glycerol to lactic acid coupled with hydrogen production over a cooperative BiOx/Au catalyst

Photoelectrocatalytic (PEC) strategy has emerged as a promising approach to drive organic reactions under mild conditions. Here, we present a protocol for PEC oxidative coupling of aromatic amines to produce aromatic azo compounds over a porous BiVO4 nanoarray (BiVO4-NA) photoanode. We describe the fabrication of BiVO4-NA photoanode and the detailed steps for the PEC oxidative coupling reaction, including key performance data of the BiVO4-NA photoanode for synthesizing azobenzene from aniline. For complete details on the use and execution of this protocol, please refer to Luo et al. (2022).1. 

https://doi.org/10.1016/j.xpro.2023.102311

Protocol for photoelectrocatalytic synthesis of aromatic azo compounds from aromatic amines

Photoelectrocatalytic activation of C-H bond in toluene by titanium dioxide-supported sub-nanometric PtO x clusters.

Photoelectrocatalytic synthesis of aromatic azo compounds over porous nanoarrays of bismuth vanadate

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