CAS: Lignin Valorization via Microscopic Reverse Biosynthesis

在化学系化学合成(SYN)项目的支持下，纽约大学的天宁雕正在开发将制浆造纸工业的废物转化为有用的化学原料的方法。这些化学产品可用作合成聚合物(塑料)和具有有用生物活性的增值复杂分子靶标(如农药、农用化学品、药品)的积木。如果成功，这一过程将提高生物质转化的整体效率，并减少生物炼油厂和造纸业产生的废物。这个想法是将生物质或木质素作为一种可持续的原料化学品来源，并作为石油化工原料的替代品。该项目为研究生和本科生提供了在有机、无机化学和绿色化学的界面上接受培训的机会。还在制定外展计划领域，以增强LGBTQ+社区成员的能力，并鼓励他们在科学、技术、工程和数学(STEM)领域追求职业生涯。通过社交媒体将艺术与化学相结合的倡议吸引了公众，并促进了更大社区对化学的兴趣。生物质转化中的一个长期挑战是木质素的选择性降解，木质素是取代芳香分子的丰富自然来源。该项目试图通过开发一种受木质素生物合成路线启发的方法来应对这一挑战，木质素生物合成路线通过一系列氧化和自由基耦合过程形成不规则的木质素聚合物。具体地说，钛(III)介导的木质素解聚工艺开始显示出良好的前景，并将从机理上进行研究和优化。还将探索电催化方法。看似可正式逆转生物合成路线的催化剂可能可用于实现木质素解聚的高选择性，鉴于国际上对用生物可再生化学原料取代石油原料的强烈兴趣，这一领域的开发已经成熟。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

With the support of the Chemical Synthesis (SYN) program in the Division of Chemistry, Tianning Diao of New York University is developing methods to convert waste from the pulp and paper industry to useful chemical feedstocks. The chemical products could be used as building blocks for the synthesis of polymers (plastics) and value-added complex molecular targets with useful biological activity (e.g. pesticides, agrochemicals, pharmaceuticals). If successful, the process would improve the overall efficiency of biomass conversion and mitigate waste generated from biorefinery and the paper industry. The idea is to use biomass or lignin as a sustainable source of feedstock chemicals and as an alternative to petroleum-based chemical feedstocks. The project provides opportunities for graduate and undergraduate students to receive training at the interface of organic, inorganic, and green chemistry. Outreach programs area also being developed to empower members of the LGBTQ+ community and encourage them to pursue a career in science, technology, engineering, and mathematics (STEM). An initiative to combine art with chemistry through social media engages the public and promotes interest in chemistry to the greater community.A standing challenge in biomass conversion is the selective degradation of lignin, an abundant natural source for substituted aromatic molecules. This project seeks to address this challenge by developing a method inspired by the biosynthesis route of lignin, which proceeds through a series of oxidation and radical coupling processes to form the irregular lignin polymer. Specificially, a Ti(III)-mediated process is beginning to show promise for lignin depolymerization, and will be studied mechanistically and optimized. Electrocatalytic methods will also be explored. Catalysts that appear to formally reverse the biosynthesis route may be exploitable to achieve high selectivity in lignin depolymerization, an area that is ripe for development given the strong international interest in replacing petroleum feedstocks with biorenewable chemical feedstocks.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.