反应中分子的Lock-to-Butterfly变化促进表面脱羧偶联
On-Surface Decarboxylation Coupling Facilitated by Lock-to-Unlock Variation of Molecules upon the Reaction
摘要：
涉及相对高的能量势垒的表面合成（OSS）由于典型的困境而仍然具有挑战性：需要牢固的分子锚以防止反应时的分子解吸，而足够的横向迁移率对于随后的偶联和组装是至关重要的。通过将分子前体锁定在基底上，然后在反应过程中将其解锁，我们提出了一种解决这一挑战的策略。证明了基于定义明确的脱羧、中间体过渡和六聚化的高产率合成，从而导致完全由新合成的大环化合物组成的扩展且有序的网络。由于其马来酰亚胺基团的空间位阻，我们获得了优先选择的耦合。这一工作为丰富OSS的反应类型和提高偶联选择性，从而提高最终产物的结构均匀性开辟了一条有前途的途径。
英文摘要：
On-surface synthesis (OSS) involving relatively high energy barriers remains challenging due to a typical dilemma: firm molecular anchor is required to prevent molecular desorption upon the reaction, whereas sufficient lateral mobility is crucial for subsequent coupling and assembly. By locking the molecular precursors on the substrate then unlocking them during the reaction, we present a strategy to address this challenge. High-yield synthesis based on well-defined decarboxylation, intermediate transition and hexamerization is demonstrated, resulting in an extended and ordered network exclusively composed of the newly-synthesized macrocyclic compound. Thanks to the steric hindrance of its maleimide group, we attain a preferential selection of the coupling. This work unlocks a promising path to enrich the reaction types and improve the coupling selectivity hence the structual homogeneity of the final product for OSS.
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