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Hydrogenases: Hydrogenases: Electrocatalysis and Electrocatalysis and Implications for Future Implications for Future Energy Technology Energy Technology Fraser Armstrong Department of Chemistry Oxford

Hydrogenases: Electrocatalysis and Implications for Future Energy Technology

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Hydrogenases: Electrocatalysis and Implications for Future Energy Technology. Fraser Armstrong Department of Chemistry Oxford. NASA uses hydrogen fuel to launch the space shuttles. H 2 (g) + O 2 (g)  H 2 O (liq) D H = -286 kJ/mol specific enthalpy -143 kJ/gram H 2. - PowerPoint PPT Presentation

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  • Hydrogenases: Electrocatalysis and Implications for Future Energy Technology Fraser ArmstrongDepartment of ChemistryOxford

  • H2(g) + O2(g) H2O (liq) DH = -286 kJ/mol

    specific enthalpy -143 kJ/gram H2NASA uses hydrogen fuel to launch the space shuttles.

  • Sunday Telegraph

    December 21 2003

  • synthesis

    from fossil fuels

    from solar

    storageenergy conversion physical(electrolysis andphotocells)biological(fermentativeand photosynthetic)chemical, cryo,compression

    combustion

    fuel cellPt catalystenzyme, organismor smart catalyst(bioinspired)The scientific challenges for afuture H2-based energy economy

  • Chemical and Engineering NewsJuly 22,2002 Volume 80, Number 29 pp. 35-39

    RENEWABLE Hydrogen bubbles form inside flask of sulfur-deprived green algae. PHOTO BY MICHAEL BARNES, UNIVERSITY OF CALIFORNIA

  • Fe-only hydrogenaseNiFe-hydrogenaseJuan Fontecilla-Camps

  • Active site of [NiFe]-hydrogenaseAn additionalO-ligand is presentin inactive states

  • ACTIVE SITE Oxford University Ph.D. student Sophie E. Lamle investigates activity of hydrogenase docked on an electrode. PHOTO BY MICHAEL FREEMANTLE

    CAN WE EXPLOIT HYDROGENASES? Insights into nature's substitute for platinum may lead to the design of inexpensive catalystsMICHAEL FREEMANTLE, C&EN LONDON

    Chemical and Engineering NewsJuly 22,2002 Volume 80, Number 29 CENEAR 80 29 pp. 35-39 ISSN 0009-2347

  • Fuel cells can be as small as we like, even micro

  • The future....fuel cells with cheap, inexpensive specific electrocatalysts, perhaps without a membrane ?ANODEHydrogenaseIdeas from Nature

  • H ........H

    Pt Pt

    H- H+

    M base

    On Pt, H2 is cleaved homolytically, Industry has to cope with CO

  • At an enzyme, H2 is cleaved heterolytically. Spectroscopic studies reveal a Ni(III)-hydrido species as an intermediate (Ni is formally oxidised by H2)III

  • H2H+Structure of [NiFe]-hydrogenasefrom Desulfovibrio gigasOther [NiFe]-hydrogenases have similar sequences or spectroscopic properties

  • a-Subunit(contains the active site)

    b-Subunit(contains the electronrelay)

    Fe

    Ni

    [4Fe-4S]prox

    [3Fe-4S]

    [4Fe-4S]dist

  • Based on flat electrode, no hydrodynamic assistance maximum current for H2 oxidation is about 4 mA/cm2 at ambient temperature and 1 bar gas (from diffusion coefficient of H2). Similar figures for O2.Power expectation is then about 4 mW/cm2, whatever the catalyst isWhat we expect from chemistry alone

  • Our mission..

    How good are hydrogenases for Electrocatalysis ?

    How do they behave on an electrode ?

    What are the challenges for their widespread technological application?

  • H2H+Measurecatalytic current= turnover rateControl chemistry by modulating electrode potential electrodesurfacehydrogenaseInvestigating hydrogenases by protein film voltammetry

  • Potential/ VoltsNormalised currentProtein Film Voltammetry: Catalytic action can produce a large current with characteristic dependence on potential At steady-state,rate is function ofpotential, not timeGuides to interpretation: Heering et al. J. Phys. Chem, B 102, 6889 (1998)Lger et al. Biochemistry 40, 11234 (2001).Lger et al. J. Phys. Chem. B. 106, 13058 (2002).Lger et al. Biochemistry 42, 8653 (2003).

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    Figures

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    0.000115

    0.00012

    0.000125

    0.00013

    0.000136

    0.000142

    0.000148

    0.000155

    0.000161

    0.000168

    0.000175

    0.000183

    0.000191

    0.000199

    0.000208

    0.000217

    0.000226

    0.000236

    0.000247

    0.000257

    0.000268

    0.00028

    0.000292

    0.000305

    0.000318

    0.000332

    0.000346

    0.000361

    0.000377

    0.000393

    0.00041

    0.000428

    0.000447

    0.000466

    0.000487

    0.000508

    0.00053

    0.000553

    0.000577

    0.000602

    0.000628

    0.000655

    0.000683

    0.000713

    0.000744

    0.000776

    0.00081

    0.000845

    0.000882

    0.00092

    0.00096

    0.001001

    0.001045

    0.00109

    0.001137

    0.001187

    0.001238

    0.001292

    0.001348

    0.001406

    0.001467

    0.001531

    0.001597

    0.001666

    0.001739

    0.001814

    0.001893

    0.001975

    0.00206

    0.002149

    0.002243

    0.00234

    0.002441

    0.002547

    0.002657

    0.002772

    0.002892

    0.003017

    0.003148

    0.003284

    0.003426

    0.003575

    0.003729

    0.003891

    0.004059

    0.004235

    0.004418

    0.004609

    0.004808

    0.005016

    0.005233

    0.005459

    0.005695

    0.005941

    0.006198

    0.006465

    0.006744

    0.007035

    0.007339

    0.007656

    0.007986

    0.008331

    0.00869

    0.009065

    0.009455

    0.009863

    0.010288

    0.010731

    0.011193

    0.011675

    0.012177

    0.012701

    0.013247

    0.013817

    0.014411

    0.01503

    0.015675

    0.016348

    0.017049

    0.017781

    0.018543

    0.019337

    0.020165

    0.021029

    0.021929

    0.022866

    0.023843

    0.024861

    0.025922

    0.027028

    0.02818

    0.029381

    0.030631

    0.031934

    0.033291

    0.034705

    0.036177

    0.037711

    0.039308

    0.040971

    0.042703

    0.044506

    0.046383

    0.048337

    0.050371

    0.052489

    0.054692

    0.056984

    0.05937

    0.061852

    0.064434

    0.067119

    0.069912

    0.072817

    0.075836

    0.078976

    0.082238

    0.085629

    0.089153

    0.092813

    0.096616

    0.100565

    0.104666

    0.108923

    0.113341

    0.117928

    0.122685

    0.12762

    0.132737

    0.138044

    0.143543

    0.149242

    0.155146

    0.161262

    0.167591

    0.174144

    0.180923

    0.187936

    0.195188

    0.202681

    0.210424

    0.218421

    0.226679

    0.235198

    0.243986

    0.253048

    0.262386

    0.272003

    0.281905

    0.292092

    0.302568

    0.313335

    0.324395

    0.335748

    0.347394

    0.359331

    0.37156

    0.38408

    0.396886

    0.409972

    0.423337

    0.436974

    0.450874

    0.465032

    0.479438

    0.49408

    0.508947

    0.524028

    0.539304

    0.554763

    0.570385

    0.586155

    0.602048

    0.618048

    0.634124

    0.650258

    0.666423

    0.682589

    0.698727

    0.714807

    0.730798

    0.746672

    0.762386

    0.777908

    0.793207

    0.80824

    0.822972

    0.837367

    0.851385

    0.864987

    0.878136

    0.890795

    0.902924

    0.914489

    0.925451

    0.93578

    0.945434

    0.954388

    0.962608

    0.97007

    0.976743

    0.982603

    0.987634

    0.99181

    0.995118

    0.997546

    0.999083

    0.999723

    0.999461

    0.998296

    0.996234

    0.993281

    0.989441

    0.984731

    0.979167

    0.972762

    0.965543

    0.957529

    0.948753

    0.939237

    0.929017

    0.918121

    0.906589

    0.894451

    0.881749

    0.868519

    0.854803

    0.840635

    0.826058

    0.811117

    0.795842

    0.780279

    0.764469

    0.748443

    0.732246

    0.71591

    0.699473

    0.68297

    0.666431

    0.649886

    0.633374

    0.616915

    0.600541

    0.584271

    0.568136

    0.552153

    0.536347

    0.520732

    0.505328

    0.49015

    0.475211

    0.460525

    0.446103

    0.431955

    0.418087

    0.40451

    0.391229

    0.378245

    0.365565

    0.353194

    0.34113

    0.329375

    0.317928

    0.306791

    0.29596

    0.285435

    0.275214

    0.265292

    0.255666

    0.246333

    0.237286

    0.228525

    0.220041

    0.211829

    0.203885

    0.196204

    0.188779

    0.181605

    0.174674

    0.167981

    0.161522

    0.155289

    0.149275

    0.143475

    0.137884

    0.132494

    0.1273

    0.122296

    0.117477

    0.112836

    0.108367

    0.104065

    0.099926

    0.095943

    0.09211

    0.088425

    0.084879

    0.08147

    0.078193

    0.075043

    0.072015

    0.069105

    0.066309

    0.063622

    0.06104

    0.058561

    0.05618

    0.053892

    0.051696

    0.049587

    0.047562

    0.045618

    0.043752

    0.041961

    0.040242

    0.038591

    0.037008

    0.035488

    0.03403

    0.03263

    0.031288

    0.03

    0.028764

    0.027579

    0.026442

    0.025351

    0.024305

    0.023301

    0.022338

    0.021416

    0.02053

    0.019681

    0.018867

    0.018086

    0.017338

    0.01662

    0.015931

    0.015271

    0.014638

    0.014032

    0.01345

    0.012892

    0.012357

    0.011845

    0.011353

    0.010882

    0.01043

    0.009997

    0.009582

    0.009184

    0.008803

    0.008437

    0.008087

    0.007751

    0.007428

    0.00712

    0.006824

    0.00654

    0.006268

    0.006008

    0.005758

    0.005518

    0.005289

    0.005069

    0.004858

    0.004656

    0.004462

    0.004277

    0.004099

    0.003928

    0.003765

    0.003608

    0.003458

    0.003314

    0.003176

    0.003044

    0.002917

    0.002796

    0.00268

    0.002568

    0.002461

    0.002359

    0.002261

    0.002166

    0.002076

    0.00199

    0.001907

    0.001828

    0.001752

    0.001679

    0.001609

    0.001542

    0.001478

    0.001416

    0.001357

    0.001301

    0.001247

    0.001195

    0.001145

    0.001097

    0.001052

    0.001008

    0.000966

    0.000926

    0.000887

    0.00085

    0.000815

    0.000781

    0.000748

    0.000717

    0.000687

    0.000659

    0.000631

    0.000605

    0.00058

    0.000556

    0.000533

    0.00051

    0.000489

    0.000469

    0.000449

    0.000431

    0.000413

    0.000395

    0.000379

    0.000363

    0.000348

    0.000334

    0.00032

    0.000306

    0.000294

    0.000281

    0.00027

    0.000259

    0.000248

    0.000237

    0.000228

    0.000218

    0.000209

    0.0002

    0.000192

    0.000184

    0.000176

    0.000169

    0.000162

    0.000155

    0.000149

    0.000143

    0.000137

    0.000131

    0.000125

    0.00012

    0.000115

    0.00011

    0.000106

    0.000101

    0.000097

    0.000093

    0.000089

    0.000086

    0.000082

    0.000079

    0.000075

    0.000072

    0.000069

    0.000066

    0.000064

    0.000061

    0.000058

    0.000056

    0.000054

    0.000051

    0.000049

    0.000047

    0.000045

    0.000043

    0.000042

    0.00004

    0.000038

    0.000037

    0.000035

    0.000034

    0.000032

    0.000031

    0.00003

    0.000028

    0.000027

    0.000026

    0.000025

    0.000024

    0.000023

    0.000022

    0.000021

    0.00002

    0.000019

    0.000019

    0.000018

    0.000017

    0.000016

    0.000016

    0.000015

    0.000014

    0.000014

    0.000013

    0.000013

    0.000012

    0.000012

    &A

    Page &P

    Potential

    Normalised Current

    2C

    0.3-0.0000120.3-0.000042-0.3-5.98203

    0.299-0.0000120.299-0.000042-0.295-5.98202

    0.298-0.0000130.298-0.000042-0.29-5.98202

    0.297-0.0000130.297-0.000044-0.285-5.98201

    0.296-0.0000140.296-0.000046-0.28-5.982

    0.295-0.0000140.295-0.000048-0.275-5.982

    0.294-0.0000150.294-0.00005-0.27-5.98198

    0.293-0.0000160.293-0.000052-0.265-5.98197

    0.292-0.0000160.292-0.000054-0.26-5.98195

    0.291-0.0000170.291-0.000056-0