Pei Lang, Luo Zhenggang, Wang Xusheng, Ma Zhanfeng, Nie Yuhang, Zhong Jiasong, Yang Ding, Bandaru Sateesh, Su Bao-Lian
College of Materials and Environmental Engineering, Hangzhou Dianzi University, Hangzhou 310018, China; Key Laboratory of Surface & Interface Science of Polymer Materials of Zhejiang Province, Hangzhou 310018, China.
College of Materials and Environmental Engineering, Hangzhou Dianzi University, Hangzhou 310018, China.
J Colloid Interface Sci. 2023 Dec 15;652(Pt A):636-645. doi: 10.1016/j.jcis.2023.07.148. Epub 2023 Jul 25.
The conversion of CO into syngas, a mixture of CO and H, via photocatalytic reduction, is a promising approach towards achieving a sustainable carbon economy. However, the evolution of highly adjustable syngas, particularly without the use of sacrifice reagents or additional cocatalysts, remains a significant challenge. In this study, a step-scheme (S-scheme) 0D ZnGaO nanodots (∼7 nm) rooted g-CN nanosheets (denoted as ZnGaO/CN) heterojunction photocatalyst was synthesized vis a facial in-situ growth strategy for efficient CO-to-syngas conversion. Both experimental and theoretical studies have demonstrated that the polymeric nature of g-CN and highly distributed ZnGaO nanodots synergistically contribute to a strong interaction between metal oxide and CN support. Furthermore, the desirable S-scheme heterojunction in ZnGaO/CN efficiently promotes charge separation, enabling strong photoredox ability. As a result, the S-scheme ZnGaO/CN exhibited remarkable activity and selectivity in photochemical conversion of CO into syngas, with a syngas production rate of up to 103.3 μ mol g h, even in the absence of sacrificial agents and cocatalyst. Impressively, the CO/H ratio of syngas can be tunable within a wide range from 1:4 to 2:1. This work exemplifies the effectiveness of a meticulously designed S-scheme heterojunction photocatalyst for CO-to-syngas conversion with adjustable composition, thus paving the way for new possibilities in sustainable energy conversion and utilization.
通过光催化还原将一氧化碳转化为合成气（一氧化碳和氢气的混合物）是实现可持续碳经济的一种有前景的方法。然而，制备高度可调的合成气，特别是在不使用牺牲试剂或额外助催化剂的情况下，仍然是一项重大挑战。在本研究中，通过一种简便的原位生长策略合成了一种阶梯式（S型）零维ZnGaO纳米点（约7纳米）根植于g-CN纳米片（记为ZnGaO/CN）的异质结光催化剂，用于高效的一氧化碳到合成气的转化。实验和理论研究均表明，g-CN的聚合物性质和高度分散的ZnGaO纳米点协同作用，有助于金属氧化物与CN载体之间形成强相互作用。此外，ZnGaO/CN中理想的S型异质结有效地促进了电荷分离，使其具有很强的光氧化还原能力。结果，即使在没有牺牲剂和助催化剂的情况下，S型ZnGaO/CN在将一氧化碳光化学转化为合成气方面也表现出显著的活性和选择性，合成气产率高达103.3 μmol g⁻¹ h⁻¹。令人印象深刻的是，合成气的CO/H比可以在1:4到2:1的宽范围内调节。这项工作例证了精心设计的S型异质结光催化剂在一氧化碳到合成气转化中具有可调节组成的有效性，从而为可持续能源转化和利用开辟了新的可能性。
