solar fuels;
photocatalysis;
artificial protein;
supramolecular chemistry;
ruthenium;
MOLECULAR-SYSTEMS;
GREEN DIMER;
HYDROGEN;
APPROXIMATION;
INHIBITORS;
MECHANISM;
CATALYSIS;
MODEL;
HOST;
D O I:
10.1021/acscatal.3c05183
中图分类号:
O64 [物理化学(理论化学)、化学物理学];
学科分类号:
070304 ;
081704 ;
摘要:
Bovine carbonic anhydrase (BCA) is an enzyme that regulates cellular pH by catalyzing CO2 hydration. In this work, we used its well-defined zinc-containing active site to host a series of four sulfonamide-functionalized ruthenium-based water oxidation catalysts Ru1 to Ru4, thereby producing four BCA-Ru1 to BCA-Ru4 artificial metalloenzymes (ArMs). The four ruthenium complexes differed either by the nature of the spectator ligand (bda(2-) or tda(2-)) bound to the catalytic center or by the length of the linker between the axially ruthenium-bound pyridine moiety and the zinc-binding sulfonamide. The two ArMs BCA-Ru1 and BCA-Ru2 were catalytically active for photocatalytic water oxidation in aqueous solution in the presence of [Ru(bpy)(3)](ClO4)(2) as a photosensitizer, Na2S2O8 as an electron acceptor, and blue light (450 nm). The most active artificial metalloenzyme, BCA-Ru1, could drive photocatalytic O-2 production at particularly low ArM concentrations (5 mu M), yielding a turnover number (TON) of 348 and a turnover frequency (TOF) of 9 min(-1) that was 1 order of magnitude higher than for the enzyme-free catalyst. A molecular dynamics study was performed to model the interaction between the ruthenium catalyst and the BCA protein. Overall, the protein scaffold modified the second coordination sphere around the catalytic center, which enhanced the activity and stability of two out of the four water oxidation catalysts in aqueous solution, modifying their pH dependence and suppressing the need for adding any organic solvents in solution. Altogether, these results demonstrate how useful artificial metalloenzymes can be for the making of artificial photosynthetic systems.
机构:
Stockholm Univ, Dept Organ Chem, Arrhenius Lab, S-10691 Stockholm, SwedenStockholm Univ, Dept Organ Chem, Arrhenius Lab, S-10691 Stockholm, Sweden
Karkas, Markus D.
Akermark, Torbjorn
论文数: 0引用数: 0
h-index: 0
机构:
Stockholm Univ, Arrhenius Lab, Dept Mat & Environm Chem, S-10691 Stockholm, SwedenStockholm Univ, Dept Organ Chem, Arrhenius Lab, S-10691 Stockholm, Sweden
Akermark, Torbjorn
Chen, Hong
论文数: 0引用数: 0
h-index: 0
机构:
Stockholm Univ, Arrhenius Lab, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden
Stockholm Univ, Berzelii Ctr EXSELENT Porous Mat, Arrhenius Lab, S-10691 Stockholm, Sweden
China Univ Geosci, Fac Mat Sci & Chem, Wuhan 430074, Peoples R ChinaStockholm Univ, Dept Organ Chem, Arrhenius Lab, S-10691 Stockholm, Sweden
Chen, Hong
Sun, Junliang
论文数: 0引用数: 0
h-index: 0
机构:
Stockholm Univ, Arrhenius Lab, Dept Mat & Environm Chem, S-10691 Stockholm, SwedenStockholm Univ, Dept Organ Chem, Arrhenius Lab, S-10691 Stockholm, Sweden
Sun, Junliang
Akermark, Bjorn
论文数: 0引用数: 0
h-index: 0
机构:
Stockholm Univ, Dept Organ Chem, Arrhenius Lab, S-10691 Stockholm, SwedenStockholm Univ, Dept Organ Chem, Arrhenius Lab, S-10691 Stockholm, Sweden
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Kim, Jinuk
Han, Wonhee
论文数: 0引用数: 0
h-index: 0
机构:
Pohang Univ Sci & Technol, Dept Life Sci, Pohang 37673, Gyeongbuk, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Han, Wonhee
Park, Taeyong
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Chem, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Park, Taeyong
Kim, Eun Jin
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Plumbline Life Sci Inc, Seoul 06552, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Kim, Eun Jin
Bang, Injin
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Columbia Univ, Dept Physiol & Cellular Biophys, Irving Med Ctr, New York, NY 10032 USASeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Bang, Injin
Lee, Hyun Sik
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Lee, Hyun Sik
Jeong, Yejing
论文数: 0引用数: 0
h-index: 0
机构:
Sungkyunkwan Univ, Sch Pharm, Suwon 16419, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Jeong, Yejing
Roh, Kyeonghwan
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Roh, Kyeonghwan
Kim, Jeesoo
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Inst for Basic Sci Korea, Ctr RNA Res, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Kim, Jeesoo
Kim, Jong-Seo
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Inst for Basic Sci Korea, Ctr RNA Res, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Kim, Jong-Seo
Kang, Chanhee
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Kang, Chanhee
Seok, Chaok
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Chem, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Seok, Chaok
Han, Jin-Kwan
论文数: 0引用数: 0
h-index: 0
机构:
Pohang Univ Sci & Technol, Dept Life Sci, Pohang 37673, Gyeongbuk, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Han, Jin-Kwan
Choi, Hee-Jung
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
机构:
Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R ChinaDalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R China
Li, Fei
Xu, Congying
论文数: 0引用数: 0
h-index: 0
机构:
Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R ChinaDalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R China
Xu, Congying
Wang, Xiaohong
论文数: 0引用数: 0
h-index: 0
机构:
Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R ChinaDalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R China
Wang, Xiaohong
Wang, Yong
论文数: 0引用数: 0
h-index: 0
机构:
Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R ChinaDalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R China
Wang, Yong
Du, Jian
论文数: 0引用数: 0
h-index: 0
机构:
Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R ChinaDalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R China
Du, Jian
Sun, Licheng
论文数: 0引用数: 0
h-index: 0
机构:
Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R China
KTH Royal Inst Technol, Sch Chem Sci & Engn, Dept Chem, S-10044 Stockholm, SwedenDalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R China
机构:
Stockholm Univ, Dept Organ Chem, Arrhenius Lab, S-10691 Stockholm, SwedenStockholm Univ, Dept Organ Chem, Arrhenius Lab, S-10691 Stockholm, Sweden
Karkas, Markus D.
Akermark, Torbjorn
论文数: 0引用数: 0
h-index: 0
机构:
Stockholm Univ, Arrhenius Lab, Dept Mat & Environm Chem, S-10691 Stockholm, SwedenStockholm Univ, Dept Organ Chem, Arrhenius Lab, S-10691 Stockholm, Sweden
Akermark, Torbjorn
Chen, Hong
论文数: 0引用数: 0
h-index: 0
机构:
Stockholm Univ, Arrhenius Lab, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden
Stockholm Univ, Berzelii Ctr EXSELENT Porous Mat, Arrhenius Lab, S-10691 Stockholm, Sweden
China Univ Geosci, Fac Mat Sci & Chem, Wuhan 430074, Peoples R ChinaStockholm Univ, Dept Organ Chem, Arrhenius Lab, S-10691 Stockholm, Sweden
Chen, Hong
Sun, Junliang
论文数: 0引用数: 0
h-index: 0
机构:
Stockholm Univ, Arrhenius Lab, Dept Mat & Environm Chem, S-10691 Stockholm, SwedenStockholm Univ, Dept Organ Chem, Arrhenius Lab, S-10691 Stockholm, Sweden
Sun, Junliang
Akermark, Bjorn
论文数: 0引用数: 0
h-index: 0
机构:
Stockholm Univ, Dept Organ Chem, Arrhenius Lab, S-10691 Stockholm, SwedenStockholm Univ, Dept Organ Chem, Arrhenius Lab, S-10691 Stockholm, Sweden
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Kim, Jinuk
Han, Wonhee
论文数: 0引用数: 0
h-index: 0
机构:
Pohang Univ Sci & Technol, Dept Life Sci, Pohang 37673, Gyeongbuk, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Han, Wonhee
Park, Taeyong
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Chem, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Park, Taeyong
Kim, Eun Jin
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Plumbline Life Sci Inc, Seoul 06552, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Kim, Eun Jin
Bang, Injin
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Columbia Univ, Dept Physiol & Cellular Biophys, Irving Med Ctr, New York, NY 10032 USASeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Bang, Injin
Lee, Hyun Sik
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Lee, Hyun Sik
Jeong, Yejing
论文数: 0引用数: 0
h-index: 0
机构:
Sungkyunkwan Univ, Sch Pharm, Suwon 16419, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Jeong, Yejing
Roh, Kyeonghwan
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Roh, Kyeonghwan
Kim, Jeesoo
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Inst for Basic Sci Korea, Ctr RNA Res, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Kim, Jeesoo
Kim, Jong-Seo
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Inst for Basic Sci Korea, Ctr RNA Res, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Kim, Jong-Seo
Kang, Chanhee
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Kang, Chanhee
Seok, Chaok
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Chem, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Seok, Chaok
Han, Jin-Kwan
论文数: 0引用数: 0
h-index: 0
机构:
Pohang Univ Sci & Technol, Dept Life Sci, Pohang 37673, Gyeongbuk, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
Han, Jin-Kwan
Choi, Hee-Jung
论文数: 0引用数: 0
h-index: 0
机构:
Seoul Natl Univ, Dept Biol Sci, Seoul 08826, South KoreaSeoul Natl Univ, Dept Biol Sci, Seoul 08826, South Korea
机构:
Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R ChinaDalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R China
Li, Fei
Xu, Congying
论文数: 0引用数: 0
h-index: 0
机构:
Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R ChinaDalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R China
Xu, Congying
Wang, Xiaohong
论文数: 0引用数: 0
h-index: 0
机构:
Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R ChinaDalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R China
Wang, Xiaohong
Wang, Yong
论文数: 0引用数: 0
h-index: 0
机构:
Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R ChinaDalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R China
Wang, Yong
Du, Jian
论文数: 0引用数: 0
h-index: 0
机构:
Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R ChinaDalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R China
Du, Jian
Sun, Licheng
论文数: 0引用数: 0
h-index: 0
机构:
Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R China
KTH Royal Inst Technol, Sch Chem Sci & Engn, Dept Chem, S-10044 Stockholm, SwedenDalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R China