Antibody Catalysis of the Oxidation of Water

Author:

Wentworth Paul1,Jones Lyn H.1,Wentworth Anita D.1,Zhu Xueyong1,Larsen Nicholas A.1,Wilson Ian A.1,Xu Xin2,Goddard William A.2,Janda Kim D.1,Eschenmoser Albert13,Lerner Richard A.1

Affiliation:

1. Departments of Chemistry and Molecular Biology and Skaggs Institute for Chemical Biology, Scripps Research Institute, 10550 North Torrey Pines Road, La Jolla, CA 92037, USA.

2. Materials and Process Simulation Center, Division of Chemistry and Chemical Engineering (MC 139-74), California Institute of Technology, Pasadena, CA 91125, USA.

3. Laboratorium für Organische Chemie, Eidgenössische Technische Hochschule (ETH) Zürich, Universitätstrasse 16, CH-8092 Zürich, Switzerland.

Abstract

Recently we reported that antibodies can generate hydrogen peroxide (H 2 O 2 ) from singlet molecular oxygen ( 1 O 2 *). We now show that this process is catalytic, and we identify the electron source for a quasi-unlimited generation of H 2 O 2 . Antibodies produce up to 500 mole equivalents of H 2 O 2 from 1 O 2 *, without a reduction in rate, and we have excluded metals or Cl as the electron source. On the basis of isotope incorporation experiments and kinetic data, we propose that antibodies use H 2 O as an electron source, facilitating its addition to 1 O 2 * to form H 2 O 3 as the first intermediate in a reaction cascade that eventually leads to H 2 O 2 . X-ray crystallographic studies with xenon point to putative conserved oxygen binding sites within the antibody fold where this chemistry could be initiated. Our findings suggest a protective function of immunoglobulins against 1 O 2 * and raise the question of whether the need to detoxify 1 O 2 * has played a decisive role in the evolution of the immunoglobulin fold.

Publisher

American Association for the Advancement of Science (AAAS)

Subject

Multidisciplinary

Reference42 articles.

1. Antibodies have the intrinsic capacity to destroy antigens

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5. This particular antibody was selected because its native crystals diffract to a higher resolution than any other published antibody (∼1.3 Å). The root mean square differences (RMSDs) of key structural parameters were compared for the 4C6 structure before and after a soak experiment with 3 mM H 2 O 2 : RMSDs of all atoms 0.412 Å; of Cα atoms 0.327 Å; of main-chain atoms 0.328 Å; of side-chain atoms 0.488 Å.

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