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SJTU & NUS’s Latest Collaborative Research on Biorefinery Published

February 25, 2021      Author:

Recently, the research teams led by associate professor Chen Xi from China-UK Low Carbon College, SJTU and Prof. Yan Ning from National University of Singapore published a research article titled "Expanding the Boundary of Biorefinery: Organonitrogen Chemicals from Biomass" in Accounts of Chemical Research (IF =20.832), a top journal in chemistry. The article presents the latest findings in synthesizing valuable organonitrogen chemicals from biomass, putting forward two main strategies to produce organonitrogen chemicals, one by converting and refining lignocellulose/waste oil biomass, the other by involving natural chitin biomass. It elaborates tailor-designed catalyst based on different biomass resources and target product, and then analyzes the relationship between the structure and the activity of catalyst as well as its reaction route and mechanism.

Synthesizing organonitrogen chemicals from biomass has become an important research field for its potential in saving fossil resources, diversifying biomass chemicals, and enhancing the economic competitiveness of biomass synthesis. As an emerging research field, producing organonitrogen chemicals from biomass is faced with both challenges and opportunities. For example, more research needs to be done in the development of new efficient catalyst, the combination of AI and chemical approaches, and separation and purification of reaction products.

Associate professor Chen Xi from China-UK Low Carbon College, SJTU and associate professor Song Jiang from Tianjin University are the co-first authors; Prof. Yan Ning from National University of Singapore is the corresponding author; and Shanghai Jiao Tong University is the first affiliation. Associate professor Chen Xi has been dedicated to the research on utilization of chitin and cellulose biomass resources and has published more than 30 SCI papers and 5 cover articles as the first author/co-author/corresponding author with. Her papers have been cited more than 2,000 times in total (according to Scopus), giving her an H-index equaling 21.

 

Source: China-UK Low Carbon College, SJTU

Translated by Zhang Wenying

Proofread by Xiao Yangning, Fu Yuhe

ABSTRACT:

Conspectus

Organonitrogen chemicals are essential in many aspects of modern life. Over 80% of the top 200 prescribed pharmaceutical products contain at least one nitrogen atom in the molecule, while all top 10 agrochemicals contain nitrogen, just to name a few. At present, the prevailing industrial processes for manufacturing organonitrogen chemicals start from nonrenewable fossil resources, but eventually we have to make these chemicals in a more sustainable manner. Biomass represents the largest renewable carbon resource on earth, which is inexpensive and widely available. Integrating biomass into the organonitrogen chemical supply chain will mitigate the carbon footprint, diversify the product stream, and enhance the economic competitiveness of biorefinery. Short-cut synthesis routes can be created for oxygen-containing organonitrogen compounds by exploiting the inherent oxygen functionalities in the biomass resources. Moreover, for nitrogen-containing biomass components such as chitin, a unique opportunity to make organonitrogen chemicals bypassing the energy-intensive Haber-Bosch ammonia synthesis process arises. Estimated at 100 billion tons of annual production in the world, chitin captures more nitrogen than the Haber-Bosch process in the form of amide functional groups in its polymer side chain.

In this Account, we intend to summarize our efforts to establish new reaction routes to synthesize valuable organonitrogen chemicals from renewable resources. Enabled by tailor-designed catalytic systems, diverse nitrogen-containing products including amines, amino acids, nitriles, and N-heterocycles have been obtained from a range of biomass feedstock either directly or via intermediate platform compounds. Two strategies to produce organonitrogen chemicals are presented. For platform chemicals derived from cellulose, hemicellulose, lignin, and lipids, which are enriched with oxygen functionalities, in particular, hydroxyl groups, the key chemistry to be developed is the catalytic transformation of hydroxyl groups into nitrogen-containing groups using NH3 as the nitrogen source. Along this line, Ru- and Ni-based heterogeneous catalysts are developed to convert alcohols to amines and/or nitriles via a thermal catalytic pathway, while CdS nanomaterials are explored to promote -OH to -NH2 conversion under visible-light irradiation. Metal-zeolite multifunctional systems are further established to enable the synthesis of N-heterocycles from O-heterocycles. The second strategy involves the use of chitin and chitin derivatives as the starting materials. Under the concept of shell biorefinery, distinctive protocols have been established to chemically transform chitin as the sole feedstock to amino sugars, amino alcohols, furanic amides, and N-heterocycles. By combining mechanochemistry with biotransformation, an integrated process to convert shrimp shell waste to complex, high-value, chiral compounds including tyrosine and l-DOPA is also demonstrated.