Biomineralization of Nanocrystalline CdS/ZnS Photocatalysts via Controlled Surface Passivation for Enhanced Hydrogen Evolution
Biomineralization of Nanocrystalline CdS/ZnS Photocatalysts via Controlled Surface Passivation for Enhanced Hydrogen Evolution
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DOI：
10.1021/acsanm.1c03997
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发表时间：
2022-01
影响因子：
5.9
通讯作者：
John Sakizadeh;J. Cline;M. Snyder;C. Kiely;S. McIntosh
中科院分区：
文献类型：
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作者：
John Sakizadeh;J. Cline;M. Snyder;C. Kiely;S. McIntosh
在异质结光催化剂的合成中使用的高温处理和有机溶剂对于大规模制造是一个挑战，这对于社会规模的影响是必要的。虽然已经证明了在更温和的条件下的合成，但所得的材料性能通常没有竞争力。在此，我们使用纯化形式的酶（胱硫醚γ-裂合酶）展示了纳米晶CdS/ZnS核/壳析氢光催化剂的受控、水相和室温生物矿化合成。光催化析氢性能测试表明，在Na 2S/Na 2SO 3牺牲剂存在下，CdS表面的可控Zn 2+钝化使其析氢活性从1300 μ mol h-1g-1提高到3200 μmol h-1g-1，与传统化学法合成的CdS/ZnS核壳型光催化剂的析氢速率相当.稳态光致发光（PL）的强度和PL寿命的测量加上能量色散X-射线光谱表明，Zn 2+钝化的生物矿化的CdS纳米晶体的表面，与钝化的程度由锌前体的浓度直接添加到合成溶液中控制。在Na 2S/Na 2SO 3牺牲剂的存在下，铂助催化剂在最高性能的CdS/ZnS光催化剂上的光沉积进一步将析氢速率提高到7200 μmol h-1g-1，建立了生物矿化作为控制合成高性能异质结析氢光催化剂的有效平台。
The high-temperature processing and organic solvents used in the synthesis of heterojunction photocatalysts is a challenge for the large-scale manufacturing that will be necessary for impact at the societal scale. While syntheses under more benign conditions have been demonstrated, the resulting material performance is often not competitive. Herein, we demonstrate the controlled, aqueous phase, and ambient temperature biomineralization-based synthesis of nanocrystalline CdS/ZnS core/shell hydrogen evolution photocatalysts using a purified form of the enzyme, cystathionine γ-lyase. Photocatalytic hydrogen evolution measurements show that controlled Zn2+-based passivation of the surface of CdS improves the hydrogen evolution activity from 1300 μmol h–1g–1to 3200 μmol h–1g–1in the presence of a Na2S/Na2SO3sacrificial reagent, which is on par with reported hydrogen evolution rates of CdS/ZnS core/shell photocatalysts synthesized through traditional chemical routes. The steady-state photoluminescence (PL) intensity and PL lifetime measurements coupled with energy-dispersive X-ray spectroscopy indicate that Zn2+passivates the surface of biomineralized CdS nanocrystals, with the extent of passivation controlled by the concentration of the zinc precursor added directly to the synthesis solution. Photodeposition of a platinum cocatalyst onto the highest-performing CdS/ZnS photocatalyst further boosts the hydrogen evolution rate to 7200 μmol h–1g–1in the presence of a Na2S/Na2SO3sacrificial reagent, establishing biomineralization as an effective platform for the controlled synthesis of high-performing heterojunction hydrogen evolution photocatalysts.