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The electrochemical conversion of low-cost precursors into high-value chemicals using renewably generated electricity is a promising approach to build up an environmentally friendly energy cycle, including a storage element. The large-scale implementation of such process can, however, only be realized by the design of cost-effective electrocatalysts with high efficiency and highest stability. Here, we report the synthesis of N and B codoped porous carbons. The constructed B-N motives combine abundant unpaired electrons and frustrated Lewis pairs (FLPs). They result in desirable performance for electrochemical N-2 reduction reaction (NRR) and electrooxidation of 5-hydroxymethylfurfural (HMF) in the absence of any metal cocatalyst. A maximum Faradaic efficiency of 15.2% with a stable NH3 production rate of 21.3 mu g h(-1) mg(-1) is obtained in NRR. Besides, 2,5-furandicarboxylic acid (FDCA) is first obtained by using non-metalbased electrocatalysts at a conversion of 71% and with yield of 57%. Gas adsorption experiments elucidate the relationship between the structure and the ability of the catalysts to activate the substrate molecules. This work opens up deep insights for the rational design of non-metal-based catalysts for potential electrocatalytic applications and the possible enhancement of their activity by the introduction of FLPs and point defects at grain boundaries.
Radical reactions have found many applications in carbohydrate chemistry, especially in the construction of carbon–carbon bonds. The formation of carbon–heteroatom bonds has been less intensively studied. This mini-review will summarize the efforts to add heteroatom radicals to unsaturated carbohydrates like endo-glycals. Starting from early examples, developed more than 50 years ago, the importance of such reactions for carbohydrate chemistry and recent applications will be discussed. After a short introduction, the mini-review is divided in sub-chapters according to the heteroatoms halogen, nitrogen, phosphorus, and sulfur. The mechanisms of radical generation by chemical or photochemical processes and the subsequent reactions of the radicals at the 1-position will be discussed. This mini-review cannot cover all aspects of heteroatom-centered radicals in carbohydrate chemistry, but should provide an overview of the various strategies and future perspectives
Radical reactions have found many applications in carbohydrate chemistry, especially in the construction of carbon–carbon bonds. The formation of carbon–heteroatom bonds has been less intensively studied. This mini-review will summarize the efforts to add heteroatom radicals to unsaturated carbohydrates like endo-glycals. Starting from early examples, developed more than 50 years ago, the importance of such reactions for carbohydrate chemistry and recent applications will be discussed. After a short introduction, the mini-review is divided in sub-chapters according to the heteroatoms halogen, nitrogen, phosphorus, and sulfur. The mechanisms of radical generation by chemical or photochemical processes and the subsequent reactions of the radicals at the 1-position will be discussed. This mini-review cannot cover all aspects of heteroatom-centered radicals in carbohydrate chemistry, but should provide an overview of the various strategies and future perspectives