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Ethylene and propylene, as essential precursors in the chemical industry, have been playing a pivotal role in the production of various value-added chemicals that find wide applications in diverse sectors, such as polymer synthesis, lithium-ion battery electrolytes, antifreeze agents and pharmaceuticals. Nevertheless, traditional methods for olefin functionalization including chlorohydrination and epoxidation involve energy-intensive steps and environment-detrimental by-products. In contrast, electrocatalysis is emerging as a promising and sustainable approach for olefin oxidation via utilizing renewable electricity. Recent advancements in energy storage and conversion technologies have intensified the research efforts toward designing efficient electrocatalysts for the selective oxidation of ethylene and propylene, highlighting the shift towards more sustainable production methods. Herein, we summarize recent progress in the electrocatalytic oxidation of ethylene and propylene, focusing on achievement in catalyst design, reaction system selection and mechanism exploration. We figure out the advantages of different oxidation methods for improved performance and discuss the various types of catalysts like noble metals, non-noble metals, metal oxides and carbon-based materials, in facilitating the electrochemical oxidation of ethylene and propylene. Finally, we also provide an overview of current challenges and problems requiring further works. [ABSTRACT FROM AUTHOR]

Photoelectrochemistry is becoming an innovative approach to organic synthesis. Generally, the current photoelectrocatalytic organic transformations suffer from limited reaction type, low conversion efficiency and poor stability. Herein, we develop efficient and stable photoelectrode materials using metal oxide protective layer, with a focus on achieving regioselective activation of amine compounds. Notably, our photoelectrochemistry process is implemented under mild reaction conditions and does not involve any directing groups, transition metals or oxidants. The results demonstrate that beyond photocatalysis and electrocatalysis, photoelectrocatalysis exhibits high efficiency, remarkable repeatability and good functional group tolerance, highlighting its great potential for applications. [ABSTRACT FROM AUTHOR]

Selective electrochemical CO2 reduction to formic acid is an appealing strategy to achieve efficient utilization of CO2. Modification of the catalytic interface with organic linkers has been proven to promote the conversion of CO2 to CO, but the highly selective generation of formic acid is still a challenge. Herein, modification of the interface of graphene oxide (GO) with amide linkages to anchor SnO2 nanoparticles is presented to catalyze the CO2 reduction reaction (CO2RR). As expected, the as-synthesized SnO2/tert-GO shows a competitive high cathodic faradaic efficiency (FE) of 84.4% for formate at −0.96 V and shows long-term stability for the CO2RR. Further, density functional theory (DFT) calculations indicated that amide linkages facilitate the conversion of CO2 to formate. [ABSTRACT FROM AUTHOR]

The electrocatalytic production of hydrogen peroxide (H 2 O 2 ) through the two-electron oxygen reduction reaction (2e - ORR) has garnered significant research attention in recent years due to its numerous appealing advantages, such as being eco-friendly and exhibiting high energy conversion efficiency. Metal-free carbon materials with specific catalytic sites have been recognized as potential electrocatalysts for 2e - ORR; however, the design of highly efficient catalysts with well-defined structures and long-term stability for large-scale H 2 O 2 production remains unsatisfactory. In this study, three covalent organic frameworks (COFs) - imine-linked LZU-1, oxazole-linked LZU-190, and thiazole-linked LZU-190(S), are successfully synthesized to explore their catalytic activity in electrocatalytic H 2 O 2 production. Among these, the carbon sites LZU-190(S) are predominantly activated by the introduced adjacent heteroatoms via electronic effects, resulting in much higher H 2 O 2 selectivity compared to the oxazole and imine linkages. This work provides new insights into developing COFs-based electrocatalysts for efficient H 2 O 2 generation., (© 2024 Wiley‐VCH GmbH.)

Photoelectrochemistry (PEC) is burgeoning as an innovative solution to organic synthesis. However, the current PEC system suffers limited reaction types and unsatisfactory performances. Herein, we employ efficient BiVO4 photoanode with tailored deposition layers for customizing two PEC approaches toward C-N and C-P formation. Notably, our process proceeds under mild reaction conditions, easily available substrates, and ultra-low potentials. Beyond photocatalysis and electrocatalysis, customized PEC offers high efficiency, good functional group tolerance, and substantial applicability for decorating drug molecules, highlighting its promising potential to enrich the synthetic toolbox for broader organic chemistry of practical applications., (© 2024 Wiley‐VCH GmbH.)

Hydrodeoxygenation of oxygen-rich molecules toward hydrocarbons is attractive yet challenging in the sustainable biomass upgrading. The typical supported metal catalysts often display unstable catalytic performances owing to the migration and aggregation of metal nanoparticles (NPs) into large sizes under harsh conditions. Here, we develop a crystal growth and post-synthetic etching method to construct hollow chromium terephthalate MIL-101 (named as HoMIL-101) with one layer of sandwiched Ru NPs as robust catalysts. Impressively, HoMIL-101@Ru@MIL-101 exhibits the excellent activity and stability for hydrodeoxygenation of biomass-derived levulinic acid to gamma-valerolactone under 50°C and 1-megapascal H 2 , and its activity is about six times of solid sandwich counterparts, outperforming the state-of-the-art heterogeneous catalysts. Control experiments and theoretical simulation clearly indicate that the enrichment of levulinic acid and H 2 by nanocavity as substrate regulator enables self-regulating the backwash of both substrates toward Ru NPs sandwiched in MIL-101 shells for promoting reaction with respect to solid counterparts, thus leading to the substantially enhanced performance.

Electrochemical CO 2 conversion to value-added multicarbon (C 2+ ) chemicals holds promise for reducing CO 2 emissions and advancing carbon neutrality. However, achieving both high conversion rate and selectivity remains challenging due to the limited active sites on catalysts for carbon-carbon (C─C) coupling. Herein, porous CuO is coated with amorphous CuSiO 3 (p-CuSiO 3 /CuO) to maximize the active interface sites, enabling efficient CO 2 reduction to C 2+ products. Significantly, the p-CuSiO 3 /CuO catalyst exhibits impressive C 2+ Faradaic efficiency (FE) of 77.8% in an H-cell at -1.2 V versus reversible hydrogen electrode in 0.1 M KHCO 3 and remarkable C 2 H 4 and C 2+ FEs of 82% and 91.7% in a flow cell at a current density of 400 mA cm -2 in 1 M KOH. In situ characterizations and theoretical calculations reveal that the active interfaces facilitate CO 2 activation and lower the formation energy of the key intermediate *OCCOH, thus promoting CO 2 conversion to C 2+ . This work provides a rational design for steering the active sites toward C 2+ products., (© 2023 Wiley‐VCH GmbH.)

Photoelectrochemistry is becoming an innovative approach to organic synthesis. Generally, the current photoelectrocatalytic organic transformations suffer from limited reaction type, low conversion efficiency and poor stability. Herein, we develop efficient and stable photoelectrode materials using metal oxide protective layer, with a focus on achieving regioselective activation of amine compounds. Notably, our photoelectrochemistry process is implemented under mild reaction conditions and does not involve any directing groups, transition metals or oxidants. The results demonstrate that beyond photocatalysis and electrocatalysis, photoelectrocatalysis exhibits high efficiency, remarkable repeatability and good functional group tolerance, highlighting its great potential for applications., (© 2023 Wiley-VCH GmbH.)