期刊
NATURE CHEMICAL BIOLOGY
卷 12, 期 12, 页码 1046-+出版社
NATURE RESEARCH
DOI: 10.1038/NCHEMBIO.2192
关键词
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资金
- UK Engineering and Physical Sciences Research Council [EP/H00338X/2]
- UK Biology and Biotechnological Sciences Research Council [BB/K010220/1]
- Marie Curie International Incoming Fellowship [PIIF-GA-2012-328085 RPSII]
- Winton Programme for the Physics of Sustainability
- VU Amsterdam
- Laserlab-Europe Consortium
- Foundation of Chemical Sciences of NWO [700.58.305]
- European Research Council [267333]
- EU FP7 project PAPETS [GA 323901]
- Royal Netherlands Academy of Arts and Sciences
- Biotechnology and Biological Sciences Research Council [BB/K010220/1] Funding Source: researchfish
- Engineering and Physical Sciences Research Council [1504802, EP/H00338X/2] Funding Source: researchfish
- BBSRC [BB/K010220/1] Funding Source: UKRI
- EPSRC [EP/H00338X/2] Funding Source: UKRI
The integration of the water-oxidation enzyme photosystem II (PSII) into electrodes allows the electrons extracted from water oxidation to be harnessed for enzyme characterization and to drive novel endergonic reactions. However, PSII continues to underperform in integrated photoelectrochemical systems despite extensive optimization efforts. Here we carried out protein-film photoelectrochemistry using spinach and Thermosynechococcus elongatus PSII, and we identified a competing charge transfer pathway at the enzyme-electrode interface that short-circuits the known water-oxidation pathway. This undesirable pathway occurs as a result of photo-induced O-2 reduction occurring at the chlorophyll pigments and is promoted by the embedment of PSII in an electron-conducting fullerene matrix, a common strategy for enzyme immobilization. Anaerobicity helps to recover the PSII photoresponse and unmasks the onset potentials relating to the Q(A)/Q(B) charge transfer process. These findings impart a fuller understanding of the charge transfer pathways within PSII and at photosystem-electrode interfaces, which will lead to more rational design of pigment-containing photoelectrodes in general.
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