Solution-Phase Synthesis of PdH0.706 Nanocubes with Enhanced Stability and Activity toward Formic Acid Oxidation

Shi, Yifeng; Schimmenti, Roberto; Zhu, Shangqian; Venkatraman, Kartik; Chen, Ruhui; Chi, Miaofang; Shao, Minhua; Mavrikakis, Manos; Xia, Younan

doi:10.1021/jacs.1c10199

Solution-Phase Synthesis of PdH_0.706 Nanocubes with Enhanced Stability and Activity toward Formic Acid Oxidation

Journal Article · Wed Feb 02 00:00:00 EST 2022 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.1c10199· OSTI ID:1876056

^[1]; ^[2]; ^[3]; Venkatraman, Kartik ^[4]; ^[5]; ^[4]; ^[3]; ^[2]; ^[6]

Georgia Institute of Technology, Atlanta, GA (United States); University of Wisconsin−Madison Department of Chemical and Biological Engineering
University of Wisconsin, Madison, WI (United States)
Hong Kong University of Science and Technology (HKUST) (Hong Kong)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Georgia Institute of Technology, Atlanta, GA (United States)
Georgia Institute of Technology, Atlanta, GA (United States); Hong Kong University of Science and Technology (HKUST) (Hong Kong)

We report palladium is one of the few metals capable of forming hydrides, with the catalytic properties being dependent on the elemental composition and spatial distribution of H atoms in the lattice. Herein, we report a facile method for the complete transformation of Pd nanocubes into a stable phase made of PdH_0.706 by treating them with aqueous hydrazine at a concentration as low as 9.2 mM. Using formic acid oxidation (FAO) as a model reaction, we systematically investigated the structure–catalytic property relationship of the resultant nanocubes with different degrees of hydride formation. The current density at 0.4 V was enhanced by four times when the nanocubes were completely converted from Pd to PdH_0.706. On the basis of a set of slab models with PdH(100) overlayers on Pd(100), we conducted density functional theory calculations to demonstrate that the degree of hybrid formation could influence both the activity and selectivity toward FAO by modulating the relative stability of formate (HCOO) and carboxyl (COOH) intermediates. Furthermore, this work provides a viable strategy for augmenting the performance of Pd-based catalysts toward various reactions without altering the loading of this scarce metal.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of Wisconsin, Madison, WI (United States)

Sponsoring Organization:: Georgia Institute of Technology; Georgia Institute of Technology; National Science Foundation; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; AC05-00OR22725; FG02-05ER15731

OSTI ID:: 1876056

Alternate ID(s):: OSTI ID: 1887695

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 6 Vol. 144; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (59)

Highly Efficient and Durable Pd Hydride Nanocubes Embedded in 2D Amorphous NiB Nanosheets for Oxygen Reduction Reaction Lu, Yizhong; Wang, Jiong; Peng, Yuecheng Advanced Energy Materials, Vol. 7, Issue 21 https://doi.org/10.1002/aenm.201700919	journal	July 2017
Nanoporous Palladium Hydride for Electrocatalytic N ₂ Reduction under Ambient Conditions Xu, Wence; Fan, Guilan; Chen, Jialiang Angewandte Chemie International Edition, Vol. 59, Issue 9 https://doi.org/10.1002/anie.201914335	journal	January 2020
How to Remove the Capping Agent from Pd Nanocubes without Destructing Their Surface Structure for the Maximization of Catalytic Activity? Shi, Yifeng; Lyu, Zhiheng; Cao, Zhenming Angewandte Chemie International Edition, Vol. 59, Issue 43 https://doi.org/10.1002/anie.202006011	journal	August 2020
Atomic Imaging of Subsurface Interstitial Hydrogen and Insights into Surface Reactivity of Palladium Hydrides Lin, Bingqing; Wu, Xi; Xie, Lin Angewandte Chemie International Edition, Vol. 59, Issue 46 https://doi.org/10.1002/anie.202006562	journal	September 2020
Surface Reconstruction of Ultrathin Palladium Nanosheets during Electrocatalytic CO ₂ Reduction Zhao, Yong; Tan, Xin; Yang, Wanfeng Angewandte Chemie International Edition, Vol. 59, Issue 48 https://doi.org/10.1002/anie.202009616	journal	September 2020
A Comprehensive Study of Formic Acid Oxidation on Palladium Nanocrystals with Different Types of Facets and Twin Defects Choi, Sang-Il; Herron, Jeffrey A.; Scaranto, Jessica ChemCatChem, Vol. 7, Issue 14 https://doi.org/10.1002/cctc.201500094	journal	April 2015
Boron Nitride‐supported Sub‐nanometer Pd ₆ Clusters for Formic Acid Decomposition: A DFT Study Schimmenti, Roberto; Cortese, Remedios; Duca, Dario ChemCatChem, Vol. 9, Issue 9 https://doi.org/10.1002/cctc.201700248	journal	March 2017
Effect of the damping function in dispersion corrected density functional theory Grimme, Stefan; Ehrlich, Stephan; Goerigk, Lars Journal of Computational Chemistry, Vol. 32, Issue 7 https://doi.org/10.1002/jcc.21759	journal	March 2011
Boosting Activity and Selectivity of CO ₂ Electroreduction by Pre‐Hydridizing Pd Nanocubes Chang, Qiaowan; Kim, Jeonghyeon; Lee, Ji Hoon Small, Vol. 16, Issue 49 https://doi.org/10.1002/smll.202005305	journal	November 2020
Electronic structure and bonding in metal hydrides, studied with photoelectron spectroscopy Riesterer, T. Zeitschrift f�r Physik B Condensed Matter, Vol. 66, Issue 4 https://doi.org/10.1007/BF01303894	journal	December 1987
The H-Pd (hydrogen-palladium) System Manchester, F. D.; San-Martin, A.; Pitre, J. M. Journal of Phase Equilibria, Vol. 15, Issue 1 https://doi.org/10.1007/BF02667685	journal	February 1994
Embedded atom method potential for hydrogen on palladium surfaces Ciufo, Ryan A.; Henkelman, Graeme Journal of Molecular Modeling, Vol. 26, Issue 12 https://doi.org/10.1007/s00894-020-04588-x	journal	November 2020
Platinum and Palladium Monolayer Electrocatalysts for Formic Acid Oxidation Liang, Zhixiu; Song, Liang; Elnabawy, Ahmed O. Topics in Catalysis, Vol. 63, Issue 7-8 https://doi.org/10.1007/s11244-020-01264-5	journal	April 2020
Synthesis of Pd nanocrystals enclosed by {100} facets and with sizes <10 nm for application in CO oxidation Jin, Mingshang; Liu, Hongyang; Zhang, Hui Nano Research, Vol. 4, Issue 1 https://doi.org/10.1007/s12274-010-0051-3	journal	October 2010
Novel hydrogen storage properties of palladium nanocrystals activated by a pentagonal cyclic twinned structure Huang, Huang; Bao, Shixiong; Chen, Qiaoli Nano Research, Vol. 8, Issue 8 https://doi.org/10.1007/s12274-015-0776-0	journal	August 2015
Characterization of palladium hydride films by electron energy loss spectroscopy and electron diffraction Liu, D. -R.; Brown, L. M. Acta Metallurgica, Vol. 36, Issue 9 https://doi.org/10.1016/0001-6160(88)90204-0	journal	September 1988
Neutron-diffraction observations on the palladium-hydrogen and palladium-deuterium systems Worsham, J. E.; Wilkinson, M. K.; Shull, C. G. Journal of Physics and Chemistry of Solids, Vol. 3, Issue 3-4 https://doi.org/10.1016/0022-3697(57)90033-1	journal	January 1957
The chemisorption of carbon monoxide on palladium single crystal surfaces: IR spectroscopic evidence for localised site adsorption Bradshaw, A. M.; Hoffmann, F. M. Surface Science, Vol. 72, Issue 3 https://doi.org/10.1016/0039-6028(78)90367-9	journal	April 1978
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Catalytic converters: state of the art and perspectives Farrauto, Robert J.; Heck, Ronald M. Catalysis Today, Vol. 51, Issue 3-4 https://doi.org/10.1016/S0920-5861(99)00024-3	journal	July 1999
HCOOH Decomposition on Sub-Nanometer Pd6 Cluster Catalysts: The Effect of Defective Boron Nitride Supports Through First Principles Schimmenti, Roberto; Mavrikakis, Manos Applied Catalysis B: Environmental, Vol. 280 https://doi.org/10.1016/j.apcatb.2020.119392	journal	January 2021
A novel approach for CO-free H production via catalytic decomposition of hydrazine Zheng, M.; Cheng, R.; Chen, X. International Journal of Hydrogen Energy, Vol. 30, Issue 10 https://doi.org/10.1016/j.ijhydene.2004.09.014	journal	August 2005
Metal hydride materials for solid hydrogen storage: A review☆ Sakintuna, B.; Lamaridarkrim, F.; Hirscher, M. International Journal of Hydrogen Energy, Vol. 32, Issue 9 https://doi.org/10.1016/j.ijhydene.2006.11.022	journal	June 2007
Stable palladium hydride as a superior anode electrocatalyst for direct formic acid fuel cells Zhang, Jiawei; Chen, Meishan; Li, Huiqi Nano Energy, Vol. 44 https://doi.org/10.1016/j.nanoen.2017.11.075	journal	February 2018
Density functional theory studies of HCOOH decomposition on Pd(111) Scaranto, Jessica; Mavrikakis, Manos Surface Science, Vol. 650 https://doi.org/10.1016/j.susc.2015.11.020	journal	August 2016
On the structure sensitivity of and CO coverage effects on formic acid decomposition on Pd surfaces Li, Sha; Rangarajan, Srinivas; Scaranto, Jessica Surface Science, Vol. 709 https://doi.org/10.1016/j.susc.2021.121846	journal	July 2021
Aloof-beam Vibrational Electron Energy-loss Spectroscopy of Adsorbate/Metal Particle Systems Venkatraman, Kartik; March, Katia; Rez, Peter Microscopy and Microanalysis, Vol. 24, Issue S1 https://doi.org/10.1017/S1431927618002799	journal	August 2018
Ligand Effect of Shape-Controlled β-Palladium Hydride Nanocrystals on Liquid-Fuel Oxidation Reactions Kabiraz, Mrinal Kanti; Kim, Jeonghyeon; Lee, Won-Jae Chemistry of Materials, Vol. 31, Issue 15 https://doi.org/10.1021/acs.chemmater.9b01561	journal	July 2019
Computational Design of Strain in Core–Shell Nanoparticles for Optimizing Catalytic Activity Moseley, Philip; Curtin, W. A. Nano Letters, Vol. 15, Issue 6 https://doi.org/10.1021/acs.nanolett.5b01154	journal	May 2015
Tailoring the Antipoisoning Performance of Pd for Formic Acid Electrooxidation via an Ordered PdBi Intermetallic Shen, Tao; Chen, Sijing; Zeng, Rui ACS Catalysis, Vol. 10, Issue 17 https://doi.org/10.1021/acscatal.0c01537	journal	August 2020
Enhanced Formic Acid Oxidation over SnO ₂ -decorated Pd Nanocubes Rettenmaier, Clara; Arán-Ais, Rosa M.; Timoshenko, Janis ACS Catalysis, Vol. 10, Issue 24 https://doi.org/10.1021/acscatal.0c03212	journal	November 2020
Ceria Nanocrystals Supporting Pd for Formic Acid Electrocatalytic Oxidation: Prominent Polar Surface Metal Support Interactions Ye, Lin; Mahadi, A. Hanif; Saengruengrit, Chalathan ACS Catalysis, Vol. 9, Issue 6 https://doi.org/10.1021/acscatal.9b00421	journal	April 2019
Enhancing the Electrocatalytic Activity of Pd/M (M = Ni, Mn) Nanoparticles for the Oxygen Reduction Reaction in Alkaline Media through Electrochemical Dealloying Lu, Xinyao; Ahmadi, Mahdi; DiSalvo, Francis J. ACS Catalysis, Vol. 10, Issue 10 https://doi.org/10.1021/acscatal.9b05499	journal	April 2020
Pt and Pd Nanoparticles Immobilized on Amine-Functionalized Zeolite: Excellent Catalysts for Hydrogenation and Heck Reactions Mandal, Saikat; Roy, Debdut; Chaudhari, Raghunath V. Chemistry of Materials, Vol. 16, Issue 19 https://doi.org/10.1021/cm0352504	journal	August 2004
Trends in Formic Acid Decomposition on Model Transition Metal Surfaces: A Density Functional Theory study Herron, Jeffrey A.; Scaranto, Jessica; Ferrin, Peter ACS Catalysis, Vol. 4, Issue 12 https://doi.org/10.1021/cs500737p	journal	November 2014
Synthesis of Stable Shape-Controlled Catalytically Active β-Palladium Hydride Zhao, Zipeng; Huang, Xiaoqing; Li, Mufan Journal of the American Chemical Society, Vol. 137, Issue 50 https://doi.org/10.1021/jacs.5b11543	journal	December 2015
Direct Observation on Reaction Intermediates and the Role of Bicarbonate Anions in CO ₂ Electrochemical Reduction Reaction on Cu Surfaces Zhu, Shangqian; Jiang, Bei; Cai, Wen-Bin Journal of the American Chemical Society, Vol. 139, Issue 44 https://doi.org/10.1021/jacs.7b10462	journal	October 2017
Structural Effects of Electrochemical Oxidation of Formic Acid on Single Crystal Electrodes of Palladium Hoshi, Nagahiro; Kida, Kaori; Nakamura, Masashi The Journal of Physical Chemistry B, Vol. 110, Issue 25 https://doi.org/10.1021/jp0608372	journal	June 2006
Insights into the Preference of CO ₂ Formation from HCOOH Decomposition on Pd Surface: A Theoretical Study Zhang, Riguang; Liu, Hongyan; Wang, Baojun The Journal of Physical Chemistry C, Vol. 116, Issue 42 https://doi.org/10.1021/jp211900z	journal	October 2012
Spectroscopic Study of the Thermal Degradation of PVP-Capped Rh and Pt Nanoparticles in H ₂ and O ₂ Environments Borodko, Yuri; Lee, Hyun Sook; Joo, Sang Hoon The Journal of Physical Chemistry C, Vol. 114, Issue 2 https://doi.org/10.1021/jp909008z	journal	December 2009
Electrochemical Behavior of Unsupported Shaped Palladium Nanoparticles Zalineeva, Anna; Baranton, Stève; Coutanceau, Christophe Langmuir, Vol. 31, Issue 5 https://doi.org/10.1021/la5025229	journal	July 2014
Avalanching strain dynamics during the hydriding phase transformation in individual palladium nanoparticles Ulvestad, A.; Welland, M. J.; Collins, S. S. E. Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms10092	journal	December 2015
Direct visualization of hydrogen absorption dynamics in individual palladium nanoparticles Narayan, Tarun C.; Hayee, Fariah; Baldi, Andrea Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14020	journal	January 2017
In situ detection of hydrogen-induced phase transitions in individual palladium nanocrystals Baldi, Andrea; Narayan, Tarun C.; Koh, Ai Leen Nature Materials, Vol. 13, Issue 12 https://doi.org/10.1038/nmat4086	journal	September 2014
Facets and vertices regulate hydrogen uptake and release in palladium nanocrystals Johnson, Noah J. J.; Lam, Brian; MacLeod, Benjamin P. Nature Materials, Vol. 18, Issue 5 https://doi.org/10.1038/s41563-019-0308-5	journal	March 2019
Palladium nanocrystals enclosed by {100} and {111} facets in controlled proportions and their catalytic activities for formic acid oxidation Jin, Mingshang; Zhang, Hui; Xie, Zhaoxiong Energy Environ. Sci., Vol. 5, Issue 4 https://doi.org/10.1039/C2EE02866B	journal	January 2012
Electrocatalysis of formic acid on palladium and platinum surfaces: from fundamental mechanisms to fuel cell applications Jiang, Kun; Zhang, Han-Xuan; Zou, Shouzhong Phys. Chem. Chem. Phys., Vol. 16, Issue 38 https://doi.org/10.1039/C4CP03151B	journal	January 2014
The effect of particle size, morphology and support on the formation of palladium hydride in commercial catalysts Parker, Stewart F.; Walker, Helen C.; Callear, Samantha K. Chemical Science, Vol. 10, Issue 2 https://doi.org/10.1039/C8SC03766C	journal	January 2019
Hydrothermal synthesis of palladium nitrides as robust multifunctional electrocatalysts for fuel cells Guo, Ruiyun; Zhang, Ke; Liu, Yaming Journal of Materials Chemistry A, Vol. 9, Issue 10 https://doi.org/10.1039/D0TA11054J	journal	January 2021
Pd nanoparticles for C–C coupling reactions Balanta, Angelica; Godard, Cyril; Claver, Carmen Chemical Society Reviews, Vol. 40, Issue 10 https://doi.org/10.1039/c1cs15195a	journal	January 2011
Electronic structure and crystal phase stability of palladium hydrides Houari, Abdesalem; Matar, Samir F.; Eyert, Volker Journal of Applied Physics, Vol. 116, Issue 17 https://doi.org/10.1063/1.4901004	journal	November 2014
Inelastic neutron scattering study on different grades of palladium of varying pretreatment Albers, P.; Poniatowski, M.; Parker, S. F. Journal of Physics: Condensed Matter, Vol. 12, Issue 20 https://doi.org/10.1088/0953-8984/12/20/301	journal	May 2000
Electronic structure and surface kinetics of palladium hydride studied with x-ray photoelectron spectroscopy and electron-energy-loss spectroscopy Bennett, P. A.; Fuggle, J. C. Physical Review B, Vol. 26, Issue 11 https://doi.org/10.1103/PhysRevB.26.6030	journal	December 1982
Self-consistent pseudopotential calculation of the electronic structure of PdH and Pd 4 H Chan, C. T.; Louie, Steven G. Physical Review B, Vol. 27, Issue 6 https://doi.org/10.1103/PhysRevB.27.3325	journal	March 1983
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Improved adsorption energetics within density-functional theory using revised Perdew-Burke-Ernzerhof functionals Hammer, B.; Hansen, L. B.; Nørskov, J. K. Physical Review B, Vol. 59, Issue 11 https://doi.org/10.1103/PhysRevB.59.7413	journal	March 1999
The Reaction of Hydrogen Atoms with Palladium and its Alloys Oates, W. A.; Flanagan, Ted B. Canadian Journal of Chemistry, Vol. 53, Issue 5 https://doi.org/10.1139/v75-097	journal	March 1975
CRC Handbook of Chemistry and Physics Haynes, W. M.; Lide, David R.; Bruno, Thomas J. CRC press https://doi.org/10.1201/9781315380476	book	June 2016
Thermal Degradation of Poly(N-vinylpyrrolidone)–Poly(vinyl alcohol) Blends Rao, Vijayalaxmi; Latha, P.; Ashokan, P. V. Polymer Journal, Vol. 31, Issue 10 https://doi.org/10.1295/polymj.31.887	journal	October 1999

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Solution-Phase Synthesis of PdH0.706 Nanocubes with Enhanced Stability and Activity toward Formic Acid Oxidation

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Solution-Phase Synthesis of PdH_0.706 Nanocubes with Enhanced Stability and Activity toward Formic Acid Oxidation