西安交通大学动力工程多相流国家重点实验室,710049,西安
收稿:2026-05-07,
修回:2026-06-23,
录用:2026-07-20,
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任杰玲, 常俏, 卢纪言, 等. 硫前驱体调控硫化非晶零价铁界面电子传递强化光发酵产氢[J/OL]. 西安交通大学学报, 2026.
REN Jieling, CHANG Qiao, LU Jiyan, et al. Sulfur Precursor-Regulated Electron Transfer in Sulfidated Amorphous Zero-Valent Iron for Enhanced Photofermentative Hydrogen Production[J/OL]. JOURNAL OF XI’AN JIAOTONG UNIVERSITY, 2026.
任杰玲, 常俏, 卢纪言, 等. 硫前驱体调控硫化非晶零价铁界面电子传递强化光发酵产氢[J/OL]. 西安交通大学学报, 2026. DOI:
REN Jieling, CHANG Qiao, LU Jiyan, et al. Sulfur Precursor-Regulated Electron Transfer in Sulfidated Amorphous Zero-Valent Iron for Enhanced Photofermentative Hydrogen Production[J/OL]. JOURNAL OF XI’AN JIAOTONG UNIVERSITY, 2026. DOI:
针对光发酵产氢过程中电子利用率低的问题,通过调控硫前驱体构建不同界面结构的硫化非晶零价铁(SAZV
I),并与荚膜红杆菌(
Rhodobacter capsulatus
)SB1003组装形成生物杂合体系。采用Na
2
S、Na
2
S
2
O
4
和K
2
S
6
对非晶零价铁进行硫化改性,通过调控Fe-S界面结构构建高效电子供体,并结合材料表征、电化学分析及响应面法评估其电子供给能力及产氢性能。结果表明,不同硫前驱体显著影响Fe-S界面构型及电子传递能力。其中,Na
2
S构建的SAZVI形成均一FeS导电层,并保留较高比例Fe
0
活性位点。XPS分析表明,Fe
0
、Fe
2+
和S
2−
物种的富集优化了界面电子结构,使材料表现出更负的腐蚀电位(-1.27 V)。基于该材料构建的杂合体系获得最佳产氢性能,累积产氢量达到2865.43 mL·L
-1
,最大产氢速率为60.24 mL·(L·h)
-1
,产氢延迟期缩短至2.78 h。响应面优化结果表明,最优条件为pH 7.53、葡萄糖浓度11 g·L
-1
和灯功率42 W。在该条件下,体系产氢量较对照组提高52.34%。本研究从界面工程角度阐明了硫前驱体调控Fe-S结构对电子传递的关键作用,为构建高效生物杂合产氢体系提供了参考。
To address the low electron utilization efficiency in photofermentative hydrogen production
sulfidated amorphous zero-valent iron (SAZVI) with different interfacial structures was synthesized by regulating sulfur precursors and subsequently assembled with
Rhodobacter capsulatus
SB1003 to construct a biohybrid system. Na
2
S
Na
2
S
2
O
4
and K
2
S
6
were employed to sulfurize amorphous zero-valent iron
enabling the construction of efficient electron donors through modulation of the Fe-S interfacial structure. Material characterization
electrochemical analyses
and response surface methodology were combined to evaluate the electron-donating capability and hydrogen-production performance of the resulting systems. The results demonstrated that sulfur precursors markedly influenced the Fe-S interfacial configuration and electron-transfer capability. Among them
the Na
2
S-derived SAZVI exhibited a uniform FeS conductive layer while retaining a high proportion of Fe
0
active sites. XPS analysis revealed that the enrichment of Fe
0
Fe
2+
and S
2−
species optimized the interfacial electronic structure
resulting in a more negative corrosion potential (-1.27 V). Accordingly
the biohybrid s
ystem constructed with Na
2
S-derived SAZVI achieved the best hydrogen-production performance
with a cumulative hydrogen yield of 2865.43 mL·L
-1
a maximum hydrogen production rate of 60.24 mL·(L·h)
-1
and a shortened lag phase of 2.78 h. Response surface optimization identified the optimal operating conditions as pH 7.53
glucose concentration of 11 g·L
-1
and lamp power of 42 W
under which hydrogen production was enhanced by 52.34% compared with the control. This study elucidates the critical role of sulfur-precursor-regulated Fe-S interfacial structures in facilitating electron transfer. It offers a reference for developing highly efficient biohybrid systems for photofermentative hydrogen production.
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