Hard-constraint physics-residual networks for hydrogen crossover prediction and high-pressure extrapolation in PEM water electrolysis
Authors: Yong-Woon Kim, Jihyeok Lee, Chulung Kang, Yung-Cheol Byun
Organizations: Department of Computer Engineering, Jeju National University, Jeju, 63243, South Korea · Faculty of Applied Energy System, Jeju National University, Jeju, 63243, South Korea · Department of Mechanical System Engineering, Jeju National University, Jeju, 63243, South Korea · Department of Computer Engineering, Major of Electronic Engineering, Jeju National University, Jeju, 63243, South Korea
Abstract
Hydrogen crossover is a critical safety and efficiency constraint in high-pressure polymer electrolyte membrane water electrolysis (PEMWE), but accurate prediction remains difficult because data are limited, transport physics are strongly coupled, and industrial operation requires reliable extrapolation beyond observed conditions. This study develops a hard-constraint physics-residual network (PR-Net) for hydrogen crossover prediction in PEMWE and compares it with a purely data-driven neural network (NN) and a soft-constraint physics-informed neural network (PINN). PR-Net embeds Henry's, Fick's, and Faraday's laws as a deterministic backbone and learns only a residual correction for unmodelled nonlinear effects. The benchmark includes 184 observations from eight peer-reviewed sources across six membrane types, covering 1-200 bar, 25−85°C, and 0.05−5.0Acm−2. PR-Net achieves R2=99.57±0.16, with 9-fold lower prediction variability than NN and PINN. In pressure-axis extrapolation, PR-Net attains R2=94.02±0.92 at 200 bar, 2.5 times beyond the training pressure range, compared with 68.06±5.52 for PINN and 58.00±8.60 for NN (p < 0.001). Residual analysis indicates that the learned correction captures part of the high-pressure gas-phase non-ideality and recovers a transport-regime transition near 0.23Acm−2 between Fickian diffusion-dominated and Faradaic production-dominated transport. With a computation time of 1.08±0.34ms on low-power embedded hardware, PR-Net provides a practical framework for real-time crossover monitoring, adaptive process control, and safer high-pressure green-hydrogen operation.
Green hydrogen plays an essential role in decarbonization, with capacity projected to scale to 560 GW by 2030 (vs. 1.39 GW in 2023) in net-zero settings. Proton exchange membrane (PEM) electrolysis is one of the most promising technology routes to green hydrogen production, and real-time system health monitoring of PEM electrolyzers is essential for their scalable deployment. In lab settings, performance degradation can be characterized through electrochemical testing protocols by periodic pauses of normal operation. Such interruption is not practical for full-scale stack deployments, limiting system operators' ability to make real-time assessments of state-of-health (SoH). We present a machine learning (ML) framework that performs virtual electrochemical characterization during normal operation. The method uses an encoder-decoder transformer, conditioned on operational data, to reconstruct characterization outputs, focusing here on polarization curves. Inspired by patch-based sequence tokenization, we segment the inputs into patches and encode them to form meaningful tokens, which substantially improves learning efficiency. Across four longitudinal runs, lasting up to 478 hours on different test cells and loading cycles, the model accurately reconstructed polarization curves and achieved 10x reduction in mean squared error (MSE) compared to a vanilla transformer. This proof-of-concept demonstrates that ML models can enable continuous performance monitoring for PEM electrolyzers and that the encoder captures meaningful latent representations of SoH, opening up opportunities to derive interpretable indicators in future work.
This study develops a dimensionless multi-domain physics-informed neural network (PINN) framework for electro-osmotic radial consolidation considering smear effects and combined vacuum and surcharge loading. Three PINN-based models are investigated: a standard soft-constrained PINN (Std-PINN), a modified gated PINN (Mod-PINN), and a modified gated PINN with hard-constraint boundary encoding (Mod-HC-PINN). The models are evaluated against FEM reference solutions under four loading cases, including constant vacuum, exponential vacuum, exponential vacuum with ramp surcharge, and exponential vacuum with cyclic haversine surcharge. The results indicate that the gated architecture applied in Mod-PINN improves the resolution of steep pressure gradients near the cathode and smear-zone interface under constant vacuum loading. Under time-dependent loading, the soft-constrained Mod-PINN shows reduced accuracy because it must learn multiple competing objectives simultaneously. The Mod-HC-PINN mitigates this issue by embedding the cathode boundary and initial conditions into the output structure, thereby reducing the optimization burden and improving physical consistency. The Mod-HC-PINN achieves MAE values of 0.43, 0.41, and 0.27 kPa for the exponential vacuum, ramp surcharge, and cyclic surcharge cases, respectively. Sensitivity analyses further demonstrate that the proposed framework remains robust across practical ranges of network architecture, collocation density, and permeability contrast.
While physics-informed neural networks (PINNs) have shown strong potential for process modeling, physical equations are only enforced as soft constraints during training, and thus, they do not guarantee constraint satisfaction at inference. We propose a framework, called piecewise-linear Karush--Kuhn--Tucker hard-constrained PINNs (PL-KKT-hPINNs), that strictly enforces nonlinear equality constraints through piecewise-linear projection. This extends the KKT-hPINN framewor, which exactly enforces linear equalities through the Karush--Kuhn--Tucker (KKT) conditions associated with orthogonally projecting neural network outputs onto the constraint feasible region. The method is demonstrated on a continuous stirred-tank reactor (CSTR) case study for both one and two inputs. Results show that PL-KKT-hPINN preserves predictive accuracy comparable to that of a standard neural network while achieving substantially lower constraint violations. In addition, the proposed model shows improved robustness in low-data regimes, yielding lower RMSE than the unconstrained neural network for limited training sample sizes. These results demonstrate that PL-KKT-hPINN provides a computationally efficient and physically consistent framework for surrogate modeling of nonlinear chemical engineering systems.
Fateme Mohammad Mohammadi, Hector Budman, Joshua L. Pulsipher