About

Graeme Henkelman is the George W. Watt Centennial Professor at the University of Texas. His contact information includes his email henkelman@utexas.edu, office location WEL 3.160, and phone number (512) 769-3180. The page indicates his role as a professor and his association with the university, but does not provide specific details about his research focus, background, or key contributions.

Research topics

• Chemistry
• Organic chemistry
• Materials science
• Inorganic chemistry
• Physical chemistry
• Nanotechnology
• Photochemistry
• Chemical engineering
• Computer Science
• Optics
• Crystallography
• Combinatorial chemistry
• Environmental chemistry
• Biology
• Metallurgy
• Biochemistry

Selected publications

• Operando Observation of Inter‐Particle Li ⁺ Transport in Layered Bimetallic Sulfides for High‐Rate Lithium‐Sulfur Batteries

  Advanced Materials · 2026-04-09

  article

  ABSTRACT The slow reaction kinetics, particularly at high rates, hinder the practical use of lithium‐sulfur batteries (LSBs). To overcome the inadequate ion transport in conventional electrodes, a two‐dimensional layered bimetallic sulfide (FeMo 2 S 4 ) as a sulfur host, creating fast ion‐conduction pathways is developed. Using a free‐standing FeMo 2 S 4 /carbon cloth cathode with a Li 2 S 6 catholyte, high‐rate performance is achieved. Crucially, in situ high‐resolution TEM directly visualized rapid inter‐particle lithium ion transport between the layered FeMo 2 S 4 flakes, offering direct evidence of enhanced kinetics. This phenomenon, combined with strong polysulfide adsorption and high catalytic activity, boosts reaction rates. The Li 2 S 6 ‐based battery delivered a high initial capacity of 1516 mAh g − 1 and outstanding stability with only 0.028% decay per cycle at 3C. This work highlights the effectiveness of layered hosts with fast ion channels and bimetallic catalysis for durable, high‐rate LSBs.

  PublisherDOI

• Interfacial electric field engineering in Ni-ZrC heterostructures for high-efficiency zinc-air batteries

  Science China Chemistry · 2026-01-04

  articleOpen access

  Abstract Developing efficient non-precious oxygen reduction reaction (ORR) catalysts remains a critical challenge. Herein, a direct current (DC) arc plasma strategy was demonstrated to construct nitrogen-doped carbon-coated Ni-ZrC heterostructured nanoparticles ((Ni/ZrC)@NC NPs) with precisely tuned interfacial built-in electric fields (BIEFs). Theoretical studies reveal that the significant work function difference (Δ Φ ) drives an asymmetric charge redistribution at the Ni-ZrC heterointerface, shifting d-band centers to optimize the adsorption energy of oxygen intermediates and to reduce reaction energy barriers. In situ optical emission spectroscopy (OES) captures the dynamic plasma evolution (electron temperature ( T e ) at local thermal equilibrium (LTE): 10,330.9 K), elucidating real-time atomic/ionic flux variations and formation mechanism of the core-shell structure and heterostructure. The synergistic Ni-ZrC core and N-doped carbon shell cooperatively enhance charge transfer kinetics and expose abundant active sites. The resulting catalyst achieves exceptional ORR activity with a half-wave potential ( E 1/2 ) of 0.82 V, surpassing Pt/C (0.80 V), alongside superior methanol tolerance and 4e − selectivity. When deployed in both liquid and all-solid-state flexible zinc-air batteries (FZABs), the catalyst delivers superior metrics: peak power densities of 251.63 mW cm −2 (liquid) and 184.22 mW cm −2 (flexible), and stable operation for a long time. This work establishes a paradigm for manipulating interfacial electronic structures via BIEFs engineering, providing a versatile platform for high-performance energy conversion technologies.

  PublisherOA PDFDOI

• Phosphine and Arsine MOFs with Stabilized Diosmium(I) Carbonyl Sawhorse Pillars

  Inorganic Chemistry · 2025-11-24

  articleCorresponding

  A new metal–organic framework (MOF) with low-valent, σ-bonded OsI–OsI pillars has been prepared using [Os2(ER3)2(μ2-O2CH)2(CO)4] sawhorse complexes (ER3 = {E(C6H4CO2)}3–; E = P or As). This is the first example of the inclusion of OsI into a MOF and is a rare example of a Lewis acidic {M–M}2+ structural motif, which provides broader insights into new synthetic methods for the preparation of MOFs containing catalytically relevant metal species. The isostructural phosphine and arsine MOFs reported here, PCM-201 and AsCM-201, respectively, achieve stabilization of the Os2 cores compared to molecular examples; combined experimental and DFT studies show that the MOF rigidity prevents cleavage of the OsI–OsI bond, which gains stability in the solid state. In contrast, UV irradiation of single crystals at 254 and 365 nm results in a release of CO ligands from OsI centers. The calculated HOMO and LUMO electronic states are found to be markedly different in the MOF versus the free complexes, in addition to significant lattice strain effects, which have important implications for the design of other low-valent MOFs for catalysis.

  PublisherDOI

• Unlocking the Potential of Phosphorus Anodes for Sodium‐Ion Batteries via Tailored Reversible Na/Polyphosphide Chemistry

  Angewandte Chemie International Edition · 2025-10-10 · 2 citations

  article

  Abstract To surmount the inherent limitations and fully harness the remarkable ultra‐high specific capacity (2,596 mAh g −1 ) of phosphorus (P) anode for sodium‐ion batteries (SIBs), we unveil an alternative fast and reversible electrochemical pathway based on Na 2 P 16 ↔Na 3 P, which transcends the barriers posed by sluggish reaction kinetics in solid‐state red P. It entails the immobilization of dissolved sodium polyphosphide (Na 2 P 16 ) onto carbon cloth (CC) matrices via robust C─O─P bonding (Na 2 P 16 @CC), and the intrinsic superior malleability of Na 2 P 16 effectively mitigates the issue of electrode pulverization caused by volumetric changes of red P during (de)sodiation. Additionally, the profound chemical adsorption of surface oxygen‐doped CC toward phosphorus species and the utilization of weakly solvating cyclic carbonate solvents synergistically inhibit the vexing dissolution of high‐order polyphosphides in the electrolyte. By capitalizing on the advances of the novel reaction mechanism, the Na 2 P 16 @CC composite anode material achieves improved sodium storage performance with a high initial reversible capacity of 1.75 mAh cm −2 at 0.1 mA cm −2 and a capacity retention of 81% over 600 cycles. This work opens an avenue toward the rational design of P‐based anodes for high‐energy SIBs.

  PublisherDOI

• Chain-Length-Selective Adsorption Governs Diffusion-Limited Dendrite Growth Mode in Battery Electrodes

  ChemRxiv · 2025-11-26

  article

  Growth of classical dendrites in metal anodes represents a far-from-equilibrium, diffusion-limited crystallization process that critically impacts the safety and performance of energy storage systems. Zn—a promising aqueous anode material—exhibits two distinct modes: continuous growth (CG), where a few crystallographically guided dendrites propagate rapidly, and independent nucleation (IN), where numerous smaller, randomly oriented dendrites form with slower propagation. Here we show that ethylene glycol–derived additives, HO–(CH2CH2O)n–H, can reliably shift growth from CG to IN. Using operando tools including optical visualization, electrochemical impedance spectroscopy, and quartz crystal microbalance, we resolve the kinetic and interfacial origins of this transition. The effect is highly chain-length dependent: PEG-400 (n ≈ 9) achieves the most efficient CG→IN shift with a threshold of 0.001 wt.% (10 ppm), while shorter or longer chains require ~1 wt.%, and no transition occurs for n <= 3 at all. Experimental measurements and quantum-chemical analysis reveals that the transition arises from two coupled processes: adsorption of PEG molecules at the electrode surface, and coordination with Zn adatoms and Zn2+ cations, which destabilize continuous growth pathways and favor repeated independent nucleation. Importantly, the shift from CG to IN reduces dendrite propagation velocity by a factor of 6. These findings establish molecular-level design rules for engineering task-specific organic molecules to control far-from-equilibrium crystallization, with direct implications for high-power batteries and electrochemical synthesis.

  PublisherDOI

• AlphaNet: scaling up local-frame-based neural network interatomic potentials

  npj Computational Materials · 2025-11-17 · 6 citations

  articleOpen access

  Molecular dynamics simulations demand an unprecedented combination of accuracy and scalability to tackle grand challenges in catalysis and materials design. To bridge this gap, we present AlphaNet, a local-frame-based equivariant model that simultaneously improves computational efficiency and predictive precision for interatomic interactions. By constructing equivariant local frames with learnable geometric transitions and enabling contractions through spatial domain and temporal domain, AlphaNet enhances the representational capacity of atomic environments, achieving state-of-the-art accuracy in energy and force predictions. Extensive benchmarks on large-scale datasets spanning molecular reactions, crystal stability, and surface catalysis (Matbench Discovery and OC2M) demonstrate its superior performance over existing neural network interatomic potentials while ensuring scalability across diverse system sizes with varying types of interatomic interactions. The synergy of accuracy, efficiency, and transferability positions AlphaNet as a transformative tool for modeling multiscale phenomena, decoding dynamics in catalysis and functional interfaces, with direct implications for accelerating the discovery of complex molecular systems and functional materials. Our code and data are available at https://github.com/zmyybc/AlphaNet .

  PublisherOA PDFDOI

• Mitigating Surface Deactivation for N₂O Abatement Using Plasma Activated Co-reactants

  ACS Catalysis · 2025-07-30 · 3 citations

  article

  Catalyst deactivation by surface bound intermediates is a persistent challenge in plasma catalysis, often limiting conversion, product selectivity, and energy efficiency in chemical processes. In this study, we identify surface oxygen accumulation (O*) as the dominant deactivation mechanism in plasma assisted nitrous oxide (N2O) decomposition and present a direct strategy to mitigate it. Using polycrystalline Cu/Al2O3 and Al2O3 catalysts under nonthermal plasma conditions, we show that Cu deactivates rapidly due to O* poisoning, as confirmed by time-resolved experiments and X-ray photoelectron spectroscopy (XPS). To counteract this, we introduce hydrogen based co-reactants (H2 and CH4) that remove surface O* by forming H2O and CO2, thereby regenerating active sites and restoring catalytic activity. This co-reactant approach enables efficient N2O decomposition at ambient temperature and pressure, conditions where traditional thermal catalysis typically requires elevated temperatures (≥300 °C) and expensive noble metals. Co-reactant addition not only enhances conversion and halves energy cost, but also, when using CH4, produces value added C2 hydrocarbons. Density functional theory calculations support these findings, revealing that co-reactants open up more favorable reaction pathways for O* removal. These results highlight how plasma catalysis creates a multidimensional design space where plasma conditions, catalyst surface chemistry, and gas phase composition can be co-optimized. This flexibility enables the use of weakly binding, earth abundant catalysts like Cu, which are otherwise inactive under mild thermal conditions. These findings demonstrate how plasma assistance can augment heterogeneous catalysis, offering alternative avenues for efficient, low temperature transformations in both environmental remediation and synthetic applications.

  PublisherDOI

• Learning from Metal Nanocrystal Heterogeneity: A Need for Information-Rich and High-Throughput Single-Nanocrystal Measurements

  ACS Nanoscience Au · 2025-07-16 · 3 citations

  reviewOpen access

  Metal nanocrystals (NCs) show utility in a variety of applications due to their unique structure-dependent properties. Isolating these structure-property relationships is crucial for NC design, but heterogeneities present in NC ensembles as well as limitations in NC characterization strategies complicate this goal. Herein, we describe the various types of intraparticle and interparticle heterogeneities common to NC ensembles and then provide a detailed description and comparison of single-particle techniques that can be used to characterize these different heterogeneities. Case studies then showcase the use of multimodal characterization approaches, where multiple, primarily single-NC techniques are used in tandem to provide new insights into metal NC structure-property relationships. We conclude with a critique of single-NC techniques that motivates the development of new high-throughput and high-resolution single-NC characterization approaches as well as computational tools, with a proposed workflow outlined to accelerate NC design and discovery.

  PublisherDOI

• Application-specific machine-learned interatomic potentials: exploring the trade-off between DFT convergence, MLIP expressivity, and computational cost

  arXiv (Cornell University) · 2025-06-06

  preprintOpen access

  Machine-learned interatomic potentials (MLIPs) are revolutionizing computational materials science and chemistry by offering an efficient alternative to {\em ab initio} molecular dynamics (MD) simulations. However, fitting high-quality MLIPs remains a challenging, time-consuming, and computationally intensive task where numerous trade-offs have to be considered, e.g., How much and what kind of atomic configurations should be included in the training set? Which level of {\em ab initio} convergence should be used to generate the training set? Which loss function should be used for fitting the MLIP? Which machine learning architecture should be used to train the MLIP? The answers to these questions significantly impact both the computational cost of MLIP training and the accuracy and computational cost of subsequent MLIP MD simulations. In this study, we use a configurationally diverse beryllium dataset and quadratic spectral neighbor analysis potential. We demonstrate that joint optimization of energy versus force weights, training set selection strategies, and convergence settings of the {\em ab initio} reference simulations, as well as model complexity can lead to a significant reduction in the overall computational cost associated with training and evaluating MLIPs. This opens the door to computationally efficient generation of high-quality MLIPs for a range of applications which demand different accuracy versus training and evaluation cost trade-offs.

  PublisherDOI

• Ternary Potassium‐Bismuth‐Telluride Intermetallic Support Promotes Electrochemical Stability in Potassium Metal Anodes

  Angewandte Chemie International Edition · 2025-06-05 · 7 citations

  articleOpen access

  Abstract We employed accumulative roll bonding to fabricate self‐standing metallurgical composite of in situ formed alkaline potassium‐bismuth‐telluride intermetallic K 2 (Bi 2/6 Te 3/6 Vac 1/6 ) embedded in potassium metal. This newly discovered thermodynamically stable potassiophilic crystal, termed “KBT”, is fcc antifluorite with K 2 Te archetype. Symmetric cells achieve 880 h of cycling at 0.5 mA cm −2 and 0.5 mAh cm −2 . Potassium metal battery (KMB) with Prussian blue (PB) cathode in carbonate electrolyte retains 80% capacity after 200 cycles at 1C. In ether‐based electrolyte with organic cathode, it achieves 80% retention after 900 cycles at 2C. Combined synchrotron X‐ray nano‐tomography, cryogenic‐focused ion beam microscopy (Cryo‐FIB) and sputter‐down X‐ray photoelectron spectroscopy (XPS) demonstrate uniform electrodeposits, versus baseline of potassium filaments intermixed with pores and coarse SEI. Binary K 3 Bi‐K and K 2 Te‐K intermetallic supports also provide improved electrochemical performance, albeit to lesser extent. Multiscale simulation provides insight into role of support structure in adatom energetics, film nucleation, early‐stage SEI morphology and interfacial stability.

  PublisherOA PDFDOI

Recent grants

• Beyond harmonic transition state theory for accelerating molecular dynamics

  NSF · $492k · 2012–2016

• CAREER: Methods for Calculating Molecular Dynamics over Long Time Scales

  NSF · $555k · 2007–2013

• Collaborative Research: CDS&E: Experimentally verified nano-oxidation simulations of Cu surfaces

  NSF · $315k · 2014–2018

• DMREF: Collaborative Research: Toolkit to Characterize and Design Bi-functional Nanoparticle Catalysts

  NSF · $700k · 2015–2018

• Computational methodology to determine rare event chemical reaction dynamics and networks

  NSF · $469k · 2018–2022

Frequent coauthors

• Hao Li

  Tohoku University

  57 shared

• Penghao Xiao

  Dalhousie University

  49 shared

• C. Buddie Mullins

  The University of Texas at Austin

  45 shared

• Richard M. Crooks

  Antrim Area Hospital

  43 shared

• Kihyun Shin

  41 shared

• Hannes Jónsson

  36 shared

• Simon M. Humphrey

  The University of Texas at Austin

  35 shared

• Naman Katyal

  The University of Texas at Austin

  33 shared

Labs

• Henkelman LabPI