Transformation of biomass and plastic wastes to value-added chemicals and fuels is considered an upcycling process that is beneficial to resource utilization. Electrocatalysis offers a sustainable approach; however, it remains a huge challenge to increase the current density and deliver market-demanded chemicals with high selectivity. Herein, we demonstrate an electrocatalytic strategy for upcycling glycerol (from biodiesel byproduct) to lactic acid and ethylene glycol (from polyethylene terephthalate waste) to glycolic acid, with both products being as valuable monomers for biodegradable polymer production. By using a nickel hydroxide-supported gold electrocatalyst (Au/Ni(OH)2), we achieve high selectivities of lactic acid and glycolic acid (77 and 91%, respectively) with high current densities at moderate potentials (317.7 mA/cm2 at 0.95 V vs RHE and 326.2 mA/cm2 at 1.15 V vs RHE, respectively). We reveal that glycerol and ethylene glycol can be enriched at the Au/Ni(OH)2 interface through their adjacent hydroxyl groups, substantially increasing local concentrations and thus high current densities. As a proof of concept, we employed a membrane-free flow electrolyzer for upcycling triglyceride and PET bottles, attaining 11.2 g of lactic acid coupled with 9.3 L of H2 and 13.7 g of glycolic acid coupled with 9.4 L of H2, respectively, revealing the potential of coproduction of valuable chemicals and H2 fuel from wastes in a sustainable fashion. 

Electrocatalytic Upcycling of Biomass and Plastic Wastes to Biodegradable Polymer Monomers and Hydrogen Fuel at High Current Densities

Atomically dispersed materials: Ideal catalysts in atomic era

Single/dual-metal atoms supported on carbon matrix can be modulated by coordination structure and neighboring active sites. Precisely designing the geometric and electronic structure and uncovering the structure-property relationships of single/dual-metal atoms confront with grand challenges. Herein, this review summarizes the latest progress in microenvironment engineering of single/dual-atom active sites via a comprehensive comparison of single-atom catalyst (SACs) and dual-atom catalysts (DACs) in term of design principles, modulation strategy, and theoretical understanding of structure-performance correlations. Subsequently, recent advances in several typical electrocatalysis process are discussed to get general understanding of the reaction mechanisms on finely-tuned SACs and DACs. Finally, full-scaled summaries of the challenges and prospects are given for microenvironment engineering of SACs and DACs. This review will provide new inspiration on the development of atomically dispersed catalysts for electrocatalytic application. This article is protected by copyright. All rights reserved.

Microenvironment Engineering of Single/Dual-atom Catalysts for Electrocatalytic Application.

As promising hydrogen energy carrier, formic acid (HCOOH) plays an indispensable role in building a complete industry chain of a hydrogen economy. Currently, the biomass upgrading assisted water electrolysis has emerged as an attractive alternative for co‐producing green HCOOH and H2 in a cost‐effective manner, yet simultaneously affording high current density and Faradaic efficiency (FE) still remains a big challenge. Here, the ternary NiVRu‐layered double hydroxides (LDHs) nanosheet arrays for selective glycerol oxidation and hydrogen evolution catalysis are reported, which yield an industry‐level 1 A cm−2 at voltage of 1.933 V, meanwhile showing considerable HCOOH and H2 productivities of 12.5 and 17.9 mmol cm−2 h−1, with FEs of almost 80% and 96%, respectively. Experimental and theoretical results reveal that the introduced Ru atoms can tune the local electronic structure of Ni‐based LDHs, which not only optimizes hydrogen adsorption kinetics for HER, but also reduces the reaction energy barriers for both the conversion of NiII into GOR‐active NiIII and carboncarbon (CC) bond cleavage. In short, this work highlights the potential of large‐scale H2 and HCOOH productions from integrated electrocatalytic system and provides new insights for designing advanced electrocatalyst for low‐cost and sustainable energy conversion.

Electrochemical Biomass Upgrading Coupled with Hydrogen Production under Industrial‐Level Current Density

The electrocatalytic splitting of water holds great promise as a sustainable and environmentally friendly technology for hydrogen production. However, the sluggish kinetics of the oxygen evolution reaction (OER) at the...

Water electrolysis for hydrogen production: from hybrid systems to self-powered/catalyzed devices

Electrochemical reduction of biomass-derived 5-hydroxymethylfurfural (HMF) represents an elegant route toward sustainable value-added chemicals production that circumvents the use of fossil fuel and hydrogen. However, the reaction efficiency is hampered by the high voltage and low activity of electrodes (Cu, Bi, Pb). Herein, we report a Ru 1 Cu single-atom alloy (SAA) catalyst with isolated Ru atoms on Cu nanowires that exhibits an electrochemical reduction of HMF to 2,5-dihydroxymethylfuran (DHMF) with promoted productivity (0.47 vs. 0.08 mmol·cm -2 ·h -1 ) and faradic efficiency (FE) (85.6 vs. 71.3%) at - 0.3 V (vs. RHE) compared with Cu counterpart. More importantly, the FE (87.5%) is largely retained at high HMF concentration (100 mM). Kinetic studies by using combined electrochemical techniques suggest disparate mechanisms over Ru 1 Cu and Cu, revealing that single-atom Ru promotes the dissociation of water to produce H* species that effectively react with HMF via an electrocatalytic hydrogenation (ECH) mechanism.

Electrocatalytic Hydrogenation of 5-Hydroxymethylfurfural Promoted by a Ru1Cu Single-Atom Alloy Catalyst.

Efficient Electrocatalytic Oxidation of Glycerol via Promoted OH* Generation over Single-Atom-Bismuth-Doped Spinel Co3O4

Plastic Waste Valorization by Leveraging Multidisciplinary Catalytic Technologies

Improving the stability of sensitive catalytic systems is an emerging research topic in the catalysis field. However, the current design of heterogeneous catalysts mainly improves their catalytic performance. This paper presents a single-atom catalyst (SAC) strategy to improve the cobalt-catalysed fluorination of acyl chlorides. A stable Co-F intermediate can be formed through the oxidative fluorination of Co1-N4@NC SAC, which can replace the unstable high-valent cobalt catalytic system and avoid the use of phosphine ligands. In the SAC system, KF can be employed as a fluorinating reagent to replace the AgF, which can be applied to various substrates and scale-up conversion with high turnover numbers (TON= 1.58 × 106). This work also shows that inorganic SACs have tremendous potential for organofluorine chemistry, and it provides a good reference for the follow-up studies on the structure-activity relationship between catalyst design and chemical reaction mechanisms.

A Single-Atom Cobalt Catalyst for the Fluorination of Acyl Chlorides at Parts-per-Million Catalyst Loading.

Styrene oxide is a pivotal organic intermediate in pharmaceuticals and fine chemicals synthesis. However, the current synthesis process relies on the use of peroxy acid or chlorohydrin, which is incompatible with establishing a more sustainable chemical industry. Here, we reported the synthesis of a quantum-sized SnO 2 on 2D graphitic carbon nitride (CN) as a heterostructured catalyst, which displays efficient photocatalytic styrene epoxidation at room temperature using O 2 as a mild oxidant, achieving styrene conversion of 98.1% and styrene oxide yield of 71.8%. Photoelectrochemical analysis demonstrates efficient electron transferring exists from CN to SnO 2 , which enhances charge carriers’ separation and transfer processes. Furthermore, we couple the photocatalytic styrene epoxidation with epoxide ring-opening amination, achieving the synthesis of value-added β-amino alcohol in a cascade reaction fashion. This work may shed light on the heterostructured catalyst design for photocatalytic selective synthesis of valuable chemicals in a sustainable manner. • 0D/2D heterojunction of SnO 2 QDs/CN composite was synthesized via impregnation and calcination methods. • SnO 2 QDs/CN shows superb photocatalytic styrene epoxidation performance. • SnO 2 QDs/CN exhibits substrate universality for cycloalkanes, norbornene and long chain alkenes. • The SnO 2 QDs play an important role in improving the separation and transfer efficiency of photocatalysts. • A two-step reaction to synthesize β-amino alcohols was designed by combining photocatalytic epoxidation of styrene with cascade epoxide ring-opening amination reaction. 

Efficient photocatalytic epoxidation of styrene over a quantum-sized SnO2 on carbon nitride as a heterostructured catalyst

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