article · ACS Catalysis
Converting lignin derivatives into high-value chemicals using light offers an environmentally friendly route to support carbon neutrality, but existing photocatalysts suffer from rapid carrier recombination and poor selectivity. To overcome these limitations, a composite photocatalyst was engineered by anchoring cerium sulphide nanoparticles onto titanium dioxide nanorods to form an S-scheme heterojunction. When tested under visible-light irradiation, the material selectively cleaved the target carbon-oxygen bond in the lignin model compound 2-phenoxy-1-acetophenone. This process yielded up to 94 per cent phenol and 80 per cent acetophenone, markedly surpassing the performance of either pure titanium dioxide or cerium sulphide alone. Theoretical calculations demonstrated that the heterojunction manages band structure and carrier dynamics effectively, improving electron-hole separation to drive the catalytic depolymerisation reaction.
Lignin is an abundant, renewable biological resource, but transforming it into valuable industrial chemicals typically demands severe, energy-intensive conditions. Developing photocatalysts that operate under visible light allows the selective breakdown of tough chemical bonds at lower energy costs. This provides a cleaner, solar-driven chemical pathway that supports broader transitions towards sustainable manufacturing and carbon-neutral bio-refineries.
This technology could eventually serve biorefinery operators and specialty chemical producers seeking to derive value from lignin waste streams by producing phenol and acetophenone. However, the technology is at an early experimental stage. Testing has been conducted exclusively on a simple model compound in laboratory conditions, meaning substantial development is required before demonstrating performance on raw, highly variable natural lignin feeds.
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In the context of achieving carbon neutrality, converting lignin-derived molecules into high-value products through photocatalytic technology provides an environmentally friendly pathway. Establishing energy-efficient processes for converting lignin derivatives requires the construction of highly active and selective photocatalysts. However, enhancing the efficiency and selectivity of photocatalysts for lignin degradation poses an ongoing challenge due to discrepancies in the redox potential and the rapid recombination of photogenerated carriers. To address these significant obstacles, we devised an innovative strategy by developing a Ce2S3 nanoparticle-anchored TiO2 nanorod (Ce2S3/TiO2). This advanced photocatalyst with the S-scheme heterojunction, enabling simultaneous control of carrier dynamics and band structure, was used to study the photocatalytic degradation of the lignin model compound 2-phenoxy-1-acetophenone. Moreover, the photocatalyst can cleave the Cβ-O-4 bond selectively to convert the lignin model compound 2-phenoxy-1-acetophenone into phenol and acetophenone under visible-light irradiation. The yields are up to 94 and 80%, respectively, and 94 or 1.4 times greater than those obtained by pure TiO2 or Ce2S3 individually. In addition, our study for the increased activity in Ce2S3/TiO2 based on density functional theory calculations emphasizes the pivotal role of the S-scheme heterojunction generated between Ce2S3 and TiO2. This heterojunction significantly enhances carrier separation efficiency, thereby augmenting the efficacy of the photocatalytic process. The findings furnish valuable insights for developing advanced photocatalytic systems tailored to the efficient depolymerization of Cβ-O-4 bonds in lignin.
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DOI: 10.1021/acscatal.4c00297
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