Hyperdimensional Brain-Inspired Learning for Phoneme Recognition With Large-Scale Inferior Colliculus Neural Activities.

OBJECTIVE: Develop a novel and highly efficient framework that decodes Inferior Colliculus (IC) neural activities for phoneme recognition. METHODS: We propose using Hyperdimensional Computing (HDC) to support an efficient phoneme recognition algorithm, in contrast to widely applied Deep Neural Networks (DNN). The high-dimensional representation and operations in HDC are rooted in human brain functionalities and naturally parallelizable, showing the potential for efficient neural activity analysis. Our proposed method includes a spatial and temporal-aware HDC encoder that effectively captures global and local patterns. As part of our framework, we deploy the lightweight HDC-based algorithm on a highly customizable and flexible hardware platform, i.e., Field Programmable Gate Arrays (FPGA), for optimal algorithm speedup. To evaluate our method, we record IC neural activities on gerbils while playing the sound of different phonemes. RESULTS: We compare our proposed method with multiple baseline machine learning algorithms in recognition quality and learning efficiency, across different hardware platforms. The results show that our method generally achieves better classification quality than the best-performing baseline. Compared to the Deep Residual Neural Network (i.e., ResNet), our method shows a speedup up to 74×, 67×, 210× on CPU, GPU, and FPGA respectively. We achieve up to 15% (10%) higher accuracy in consonant (vowel) classification than ResNet. CONCLUSION: By leveraging brain-inspired HDC for IC neural activity encoding and phoneme classification, we achieve orders of magnitude runtime speedup while improving accuracy in various challenging task settings. SIGNIFICANCE: Decoding IC neural activities is an important step to enhance understanding about human auditory system. However, these responses from the central auditory system are noisy and contain high variance, demanding large-scale datasets and iterative model fine-tuning. The proposed HDC-based framework is more scalable and viable for future real-world deployment thanks to its fast training and overall better quality.

Microstructure and Biomechanical Properties in Selective Laser Melting of Porous Metal Implants.

Two kinds of porous structure design strategies, ring-support (RS) and column-support (CS), are proposed for human implants. The accurate design of porosity is realized by adjusting the pore characteristics, such as strut diameter, pore diameter, and unit size. Porous specimens with porosity of 50%, 60%, 70%, and 80% were prepared by selective laser melting. The three-dimensional pore structure is basically consistent with the design characteristics, and the measured porosity is slightly lower than design value. The microstructure, microhardness, and friction and wear properties of the samples were studied. The results show that the performance along the scanning orientation is slightly better than that along the forming orientation. The compression and dynamic elastic modulus of porous specimens with different structures and porosities were analyzed. The CS porous with 60-80% porosity has suitable compressive strength and elastic modulus, which is close to that of human tissue, and effectively avoids the stress shielding phenomenon.

Hydration behaviors of nonfouling zwitterionic materials.

Zwitterionic materials have emerged as highly effective ultralow fouling materials for many applications, however the underlying mechanism of fouling resistance remains unclear. Using ab initio molecular dynamics simulations and surface-sensitive sum frequency generation vibrational spectroscopy, we studied the hydration behaviors of zwitterionic materials, including trimethylamine-N-oxide (TMAO) and carboxybetaines of different charge-separation distances, to understand their fouling-resistant mechanism and provide a design principle for improved performance. Our study reveals that the interplay among hydrogen bonding, net charge, and dipole moment is crucial to the fouling-resistant capabilities of zwitterionic materials. Shortening of the zwitterionic spacing strengthens hydrogen bonding with water against biomolecule attachment due to the increased electrostatic and induction interactions, charge transfer, and improved structural stability. Moreover, the shortened charge separation reduces the dipole moment of zwitterionic materials with an intrinsic near-neutral net charge, decreasing their electrostatic and dipole-dipole interactions with biofoulers, and increasing their resistance to fouling. Compared to carboxybetaine compounds, TMAO has the shortest zwitterionic spacing and exhibits the strongest hydrogen bonding, the smallest net charge, and the minimum dipole moment, making it an excellent nonfouling material.

Orientational Coupling of Molecules at Interfaces Revealed by Two-Dimensional Electronic-Vibrational Sum Frequency Generation (2D-EVSFG).

Photoinduced relaxation processes at interfaces are intimately related to many fields such as solar energy conversion, photocatalysis, and photosynthesis. Vibronic coupling plays a key role in the fundamental steps of the interface-related photoinduced relaxation processes. Vibronic coupling at interfaces is expected to be different from that in bulk due to the unique environment. However, vibronic coupling at interfaces has not been well understood due to the lack of experimental tools. We have recently developed a two-dimensional electronic-vibrational sum frequency generation (2D-EVSFG) for vibronic coupling at interfaces. In this work, we present orientational correlations in vibronic couplings of electronic and vibrational transition dipoles as well as the structural evolution of photoinduced excited states of molecules at interfaces with the 2D-EVSFG technique. We used malachite green molecules at the air/water interface as an example, to be compared with those in bulk revealed by 2D-EV. Together with polarized VSFG and ESHG experiments, polarized 2D-EVSFG spectra were used to extract relative orientations of an electronic transition dipole and vibrational transition dipoles at the interface. Combined with molecular dynamics calculations, time-dependent 2D-EVSFG data have demonstrated that structural evolutions of photoinduced excited states at the interface have different behaviors than those in bulk. Our results showed that photoexcitation leads to intramolecular charge transfer but no conical interactions in 25 ps. Restricted environment and orientational orderings of molecules at the interface are responsible for the unique features of vibronic coupling.

The DRD2 Antagonist Haloperidol Mediates Autophagy-Induced Ferroptosis to Increase Temozolomide Sensitivity by Promoting Endoplasmic Reticulum Stress in Glioblastoma.

PURPOSE: Temozolomide resistance remains a major obstacle in the treatment of glioblastoma (GBM). The combination of temozolomide with another agent could offer an improved treatment option if it could overcome chemoresistance and prevent side effects. Here, we determined the critical drug that cause ferroptosis in GBM cells and elucidated the possible mechanism by which drug combination overcomes chemoresistance. EXPERIMENTAL DESIGN: Haloperidol/temozolomide synergism was assessed in GBM cell lines with different dopamine D2 receptor (DRD2) expression in vitro and in vivo. Inhibitors of ferroptosis, autophagy, endoplasmic reticulum (ER) stress and cyclic adenosine monophosphate (cAMP)/protein kinase A (PKA) were used to validate the specific mechanisms by which haloperidol and temozolomide induce ferroptosis in GBM cells. RESULTS: In the present work, we demonstrate that the DRD2 level is increased by temozolomide in a time-dependent manner and is inversely correlated with temozolomide sensitivity in GBM. The DRD2 antagonist haloperidol, a butylbenzene antipsychotic, markedly induces ferroptosis and effectively enhances temozolomide efficacy in vivo and in vitro. Mechanistically, haloperidol suppressed the effect of temozolomide on cAMP by antagonizing DRD2 receptor activity, and the increases in cAMP/PKA triggered ER stress, which led to autophagy and ferroptosis. Furthermore, elevated autophagy mediates downregulation of FTH1 expression at the posttranslational level in an autophagy-dependent manner and ultimately leads to ferroptosis. CONCLUSIONS: Our results provide experimental evidence for repurposing haloperidol as an effective adjunct therapy to inhibit adaptive temozolomide resistance to enhance the efficacy of chemoradiotherapy in GBM, a strategy that may have broad prospects for clinical application.

Fe-Fe Double-Atom Catalysts for Murine Coronavirus Disinfection: Nonradical Activation of Peroxides and Mechanisms of Virus Inactivation.

Peroxides find broad applications for disinfecting environmental pathogens particularly in the COVID-19 pandemic; however, the extensive use of chemical disinfectants can threaten human health and ecosystems. To achieve robust and sustainable disinfection with minimal adverse impacts, we developed Fe single-atom and Fe-Fe double-atom catalysts for activating peroxymonosulfate (PMS). The Fe-Fe double-atom catalyst supported on sulfur-doped graphitic carbon nitride outperformed other catalysts for oxidation, and it activated PMS likely through a nonradical route of catalyst-mediated electron transfer. This Fe-Fe double-atom catalyst enhanced PMS disinfection kinetics for inactivating murine coronaviruses (i.e., murine hepatitis virus strain A59 (MHV-A59)) by 2.17-4.60 times when compared to PMS treatment alone in diverse environmental media including simulated saliva and freshwater. The molecular-level mechanism of MHV-A59 inactivation was also elucidated. Fe-Fe double-atom catalysis promoted the damage of not only viral proteins and genomes but also internalization, a key step of virus lifecycle in host cells, for enhancing the potency of PMS disinfection. For the first time, our study advances double-atom catalysis for environmental pathogen control and provides fundamental insights of murine coronavirus disinfection. Our work paves a new avenue of leveraging advanced materials for improving disinfection, sanitation, and hygiene practices and protecting public health.

Transformation of Graphitic Carbon Nitride by Reactive Chlorine Species: "Weak" Oxidants Are the Main Players.

Graphitic carbon nitride (g-C3N4) nanomaterials hold great promise in diverse applications; however, their stability in engineering systems and transformation in nature are largely underexplored. We evaluated the stability, aging, and environmental impact of g-C3N4 nanosheets under the attack of free chlorine and reactive chlorine species (RCS), a widely used oxidant/disinfectant and a class of ubiquitous radical species, respectively. g-C3N4 nanosheets were slowly oxidized by free chlorine even at a high concentration of 200-1200 mg L-1, but they decomposed rapidly when ClO· and/or Cl2•- were the key oxidants. Though Cl2•- and ClO· are considered weaker oxidants in previous studies due to their lower reduction potentials and slower reaction kinetics than ·OH and Cl·, our study highlighted that their electrophilic attack efficacy on g-C3N4 nanosheets was on par with ·OH and much higher than Cl·. A trace level of covalently bonded Cl (0.28-0.55 at%) was introduced to g-C3N4 nanosheets after free chlorine and RCS oxidation. Our study elucidates the environmental fate and transformation of g-C3N4 nanosheets, particularly under the oxidation of chlorine-containing species, and it also provides guidelines for designing reactive, robust, and safe nanomaterials for engineering applications.

Environmental application of chlorine-doped graphitic carbon nitride: Continuous solar-driven photocatalytic production of hydrogen peroxide.

Solar-driven photocatalytic generation of H2O2 over metal-free catalysts is a sustainable approach for value-added chemical production. Here, we synthesized chlorine-doped graphitic carbon nitride (Cl-doped g-C3N4) through a solvothermal method to effectively produce H2O2 with a rate of 1.19 ± 0.06 µM min-1 under visible light irradiation, which was improved by 104 times compared to pristine g-C3N4. Continuous net production of H2O2 was realized at a rate of 2.78 ± 0.10 µM min-1 up to 54 h with isopropanol as the hole scavenger, whereas H2O2 production was only sustained for ~ 6 h without scavengers. Both molecular simulations and advanced spectroscopic characterizations elucidated that the Cl dopant increased the charge transfer rate, decreased the bandgap, and reduced the activation energy of the rate-limiting step of O2 reduction, all of which favored H2O2 production. This work implemented a novel metal-free photocatalyst for sustainable H2O2 production and elucidated the mechanism for promoting H2O2 production that can guide future photoreactive nanomaterial design.

Radical-Driven Decomposition of Graphitic Carbon Nitride Nanosheets: Light Exposure Matters.

Understanding the transformation of graphitic carbon nitride (g-C3N4) is essential to assess nanomaterial robustness and environmental risks. Using an integrated experimental and simulation approach, our work has demonstrated that the photoinduced hole (h+) on g-C3N4 nanosheets significantly enhances nanomaterial decomposition under •OH attack. Two g-C3N4 nanosheet samples D and M2 were synthesized, among which M2 had more pores, defects, and edges, and they were subjected to treatments with •OH alone and both •OH and h+. Both D and M2 were oxidized and released nitrate and soluble organic fragments, and M2 was more susceptible to oxidation. Particularly, h+ increased the nitrate release rate by 3.37-6.33 times even though the steady-state concentration of •OH was similar. Molecular simulations highlighted that •OH only attacked a limited number of edge-site heptazines on g-C3N4 nanosheets and resulted in peripheral etching and slow degradation, whereas h+ decreased the activation energy barrier of C-N bond breaking between heptazines, shifted the degradation pathway to bulk fragmentation, and thus led to much faster degradation. This discovery not only sheds light on the unique environmental transformation of emerging photoreactive nanomaterials but also provides guidelines for designing robust nanomaterials for engineering applications.

Two-dimensional electronic-vibrational sum frequency spectroscopy for interactions of electronic and nuclear motions at interfaces.

Interactions of electronic and vibrational degrees of freedom are essential for understanding excited-states relaxation pathways of molecular systems at interfaces and surfaces. Here, we present the development of interface-specific two-dimensional electronic-vibrational sum frequency generation (2D-EVSFG) spectroscopy for electronic-vibrational couplings for excited states at interfaces and surfaces. We demonstrate this 2D-EVSFG technique by investigating photoexcited interface-active (E)-4-((4-(dihexylamino) phenyl)diazinyl)-1-methylpyridin-1- lum (AP3) molecules at the air-water interface as an example. Our 2D-EVSFG experiments show strong vibronic couplings of interfacial AP3 molecules upon photoexcitation and subsequent relaxation of a locally excited (LE) state. Time-dependent 2D-EVSFG experiments indicate that the relaxation of the LE state, S2, is strongly coupled with two high-frequency modes of 1,529.1 and 1,568.1 cm-1 Quantum chemistry calculations further verify that the strong vibronic couplings of the two vibrations promote the transition from the S2 state to the lower excited state S1 We believe that this development of 2D-EVSFG opens up an avenue of understanding excited-state dynamics related to interfaces and surfaces.

Fe-based single-atom catalysis for oxidizing contaminants of emerging concern by activating peroxides.

We prepared a single-atom Fe catalyst supported on an oxygen-doped, nitrogen-rich carbon support (SAFe-OCN) for degrading a broad spectrum of contaminants of emerging concern (CECs) by activating peroxides such as peroxymonosulfate (PMS). In the SAFe-OCN/PMS system, most selected CECs were amenable to degradation and high-valent Fe species were present for oxidation. Moreover, SAFe-OCN showed excellent performance for contaminant degradation in complex water matrices and high stability in oxidation. Specifically, SAFe-OCN, with a catalytic center of Fe coordinated with both nitrogen and oxygen (FeNxO4-x), showed 5.13-times increased phenol degradation kinetics upon activating PMS compared to the catalyst where Fe was only coordinated with nitrogen (FeN4). Molecular simulations suggested that FeNxO4-x, compared to FeN4, was an excellent multiple-electron donor and it could potential-readily form high-valent Fe species upon oxidation. In summary, the single-atom Fe catalyst enables efficient, robust, and sustainable water and wastewater treatment, and molecular simulations highlight that the electronic nature of Fe could play a key role in determining the activity of the single-atom catalyst.

A Carbon Composite Film with Three-Dimensional Reticular Structure for Electromagnetic Interference Shielding and Electro-Photo-Thermal Conversion.

The design of flexible wearable electronic devices that can shield electromagnetic waves and work in all weather conditions remains a challenge. We present in this work a low-cost technology to prepare an ultra-thin carbon fabric-graphene (CFG) composite film with outstanding electromagnetic interference shielding effectiveness (EMI SE) and electro-photo-thermal effect. The compatibility between flexible carbon fabric skeleton and brittle pure graphene matrix empowers this CFG film with adequate flexibility. The reticular fibers and porous structures play a vital role in multiple scattering and absorption of electromagnetic waves. In the frequency range of 30-1500 MHz, the CFG film can achieve a significantly high EMI SE of about 46 dB at tiny thickness (0.182 mm) and density (1.4 g cm-3) predominantly by absorption. At low safe voltages or only in sunlight, the film can self-heat to its saturation value rapidly in 40 s. Once the electricity or light supply is stopped, it can quickly dissipate heat in tens of seconds. A combination of the EMI SE and the prominent electro-photo-thermal effect further enables such a remarkable EMI shielding film to have more potential applications for communication devices in extreme zones.

Symmetry-Breaking Enhanced Herzberg-Teller Effect with Brominated Polyacenes.

Molecular symmetry is vital to the selection rule of vibrationally resolved electronic transition, particularly when the nuclear dependence of electronic wave function is explicitly treated by including Franck-Condon (FC) factor, Franck-Condon/Herzberg-Teller (FC/HT) interference, and Herzberg-Teller (HT) coupling. Our present study investigated the light absorption spectra of highly symmetric tetracene, pentacene, and hexacene molecules of point-group D2h, as well as their monobrominated derivatives with a lower Cs symmetry. It was found that the symmetry-breaking monobromination allows more vibrational normal modes and their pairs to contribute to FC/HT interference and HT coupling, respectively. Through a projection of a molecule's vibrational normal modes to its irreducible representations, a linear relationship between the FC/HT intensity to the polyacene's size was deduced alongside a quadratic dependence of the HT intensity. Both theoretically derived correlations were well justified by our numerical simulations, which also demonstrated an approximately 20% improvement on the agreement with experimental line shape if the HT theory is adopted to replace the FC approximation. Moreover, for these low-symmetry monobrominated polyacenes, the FC intensity was even weaker than its FC/HT and HT counterparts at some excitation energies, making the HT theory imperative to decipher vibronic coupling, a fundamental driving force behind numerous chemical, biological, and photophysical processes.

Singlet Fission Driven by Anisotropic Vibronic Coupling in Single-Crystalline Pentacene.

Vibronic coupling is believed to play an important role in siglet fission, wherein a photoexcited singlet exciton is converted into two triplet excitons. In the present study, we examine the role of vibronic coupling in singlet fission using polarized transient absorption microscopy and ab initio simulations on single-crystalline pentacene. It was found that singlet fission in pentacene is greatly facilitated by the vibrational coherence of a 35.0 cm-1 phonon, where anisotropic coherence persists extensively for a few picoseconds. This coherence-preserving phonon that drives the anisotropic singlet fission is made possible by a unique cross-axial charge-transfer intermediate state. In the same fashion, this phonon was also found to predominantly drive the quantum decohence of a correlated triplet pair to form a decoupled triplet dimer. Moreover, our transient kinetic experimental data illustrates notable directional anisotropicity of the singlet fission rate in single-crystalline pentacene.

Herzberg-Teller Effect on the Vibrationally Resolved Absorption Spectra of Single-Crystalline Pentacene at Finite Temperatures.

The line shape of an electronic spectrum conveys the coupling between electronic and vibrational degrees of freedom. In the present study, the light absorption spectra of single-crystalline pentacene were measured by polarized UV-vis microscopy at 77, 185, and 293 K. The vibronic coupling encoded in each spectrum was resolved by the Herzberg-Teller theory that considers the contributions from the Franck-Condon (FC) factor, Franck-Condo/Herzberg-Teller (FC/HT) interference, and Herzberg-Teller (HT) coupling. Specifically, excitation energies, electronic transition dipole moments, and their nuclear gradients were evaluated by the GW method to ensure numerical accuracy, while the computationally efficient density function theory was employed to determine the optimized structures and vibrational normal modes. For every pair of electronic transition and normal mode that gives rise to a strong vibronic transition intensity, we examined their spatial characteristics by projecting them onto the three crystal axes. It was found that all normal modes strongly coupled to the lowest-lying a-polarized electronic transitions oscillate along axis a, whereas none of their counterparts for the lowest-lying b-polarized electronic transitions is predominantly along axis b. This notable difference on the alignment between the electronic transition and molecular vibration could help the directional control of charge dissociation and/or spin separation. Moreover, a significant variance of the destructive FC/HT interference was discovered with increasing temperatures that can well explain the a-polarized fading tableland near 650 nm. Finally, the importance of HT coupling was corroborated by comparing its intensity with those of FC factor and FC/HT interference. Taken all together, the vibrational dependence of the electronic wave function is critical to resolve the light absorption spectra of single-crystalline pentacene and its temperature effects, facilitating the systematic design of functional optical materials based on pentacene and its derivatives.

Anisotropic Singlet Fission in Single Crystalline Hexacene.

Singlet fission is known to improve solar energy utilization by circumventing the Shockley-Queisser limit. The two essential steps of singlet fission are the formation of a correlated triplet pair and its subsequent quantum decoherence. However, the mechanisms of the triplet pair formation and decoherence still remain elusive. Here we examined both essential steps in single crystalline hexacene and discovered remarkable anisotropy of the overall singlet fission rate along different crystal axes. Since the triplet pair formation emerges on the same timescale along both crystal axes, the quantum decoherence is likely responsible for the directional anisotropy. The distinct quantum decoherence rates are ascribed to the notable difference on their associated energy loss according to the Redfield quantum dissipation theory. Our hybrid experimental/theoretical framework will not only further our understanding of singlet fission, but also shed light on the systematic design of new materials for the third-generation solar cells.

Biomimicry of symbiotic multi-species coevolution for discrete and continuous optimization in RFID networks.

In recent years, symbiosis as a rich source of potential engineering applications and computational model has attracted more and more attentions in the adaptive complex systems and evolution computing domains. Inspired by different symbiotic coevolution forms in nature, this paper proposed a series of multi-swarm particle swarm optimizers called PS2Os, which extend the single population particle swarm optimization (PSO) algorithm to interacting multi-swarms model by constructing hierarchical interaction topologies and enhanced dynamical update equations. According to different symbiotic interrelationships, four versions of PS2O are initiated to mimic mutualism, commensalism, predation, and competition mechanism, respectively. In the experiments, with five benchmark problems, the proposed algorithms are proved to have considerable potential for solving complex optimization problems. The coevolutionary dynamics of symbiotic species in each PS2O version are also studied respectively to demonstrate the heterogeneity of different symbiotic interrelationships that effect on the algorithm's performance. Then PS2O is used for solving the radio frequency identification (RFID) network planning (RNP) problem with a mixture of discrete and continuous variables. Simulation results show that the proposed algorithm outperforms the reference algorithms for planning RFID networks, in terms of optimization accuracy and computation robustness.

A novel comprehensive learning artificial bee colony optimizer for dynamic optimization biological problems.

There are many dynamic optimization problems in the real world, whose convergence and searching ability is cautiously desired, obviously different from static optimization cases. This requires an optimization algorithm adaptively seek the changing optima over dynamic environments, instead of only finding the global optimal solution in the static environment. This paper proposes a novel comprehensive learning artificial bee colony optimizer (CLABC) for optimization in dynamic environments problems, which employs a pool of optimal foraging strategies to balance the exploration and exploitation tradeoff. The main motive of CLABC is to enrich artificial bee foraging behaviors in the ABC model by combining Powell's pattern search method, life-cycle, and crossover-based social learning strategy. The proposed CLABC is a more bee-colony-realistic model that the bee can reproduce and die dynamically throughout the foraging process and population size varies as the algorithm runs. The experiments for evaluating CLABC are conducted on the dynamic moving peak benchmarks. Furthermore, the proposed algorithm is applied to a real-world application of dynamic RFID network optimization. Statistical analysis of all these cases highlights the significant performance improvement due to the beneficial combination and demonstrates the performance superiority of the proposed algorithm.

Dynamic population artificial bee colony algorithm for multi-objective optimal power flow.

This paper proposes a novel artificial bee colony algorithm with dynamic population (ABC-DP), which synergizes the idea of extended life-cycle evolving model to balance the exploration and exploitation tradeoff. The proposed ABC-DP is a more bee-colony-realistic model that the bee can reproduce and die dynamically throughout the foraging process and population size varies as the algorithm runs. ABC-DP is then used for solving the optimal power flow (OPF) problem in power systems that considers the cost, loss, and emission impacts as the objective functions. The 30-bus IEEE test system is presented to illustrate the application of the proposed algorithm. The simulation results, which are also compared to nondominated sorting genetic algorithm II (NSGAII) and multi-objective ABC (MOABC), are presented to illustrate the effectiveness and robustness of the proposed method.

Visible-Light-Responsive Graphitic Carbon Nitride: Rational Design and Photocatalytic Applications for Water Treatment.

Graphitic carbon nitride (g-C3N4) has recently emerged as a promising visible-light-responsive polymeric photocatalyst; however, a molecular-level understanding of material properties and its application for water purification were underexplored. In this study, we rationally designed nonmetal doped, supramolecule-based g-C3N4 with improved surface area and charge separation. Density functional theory (DFT) simulations indicated that carbon-doped g-C3N4 showed a thermodynamically stable structure, promoted charge separation, and had suitable energy levels of conduction and valence bands for photocatalytic oxidation compared to phosphorus-doped g-C3N4. The optimized carbon-doped, supramolecule-based g-C3N4 showed a reaction rate enhancement of 2.3-10.5-fold for the degradation of phenol and persistent organic micropollutants compared to that of conventional, melamine-based g-C3N4 in a model buffer system under the irradiation of simulated visible sunlight. Carbon-doping but not phosphorus-doping improved reactivity for contaminant degradation in agreement with DFT simulation results. Selective contaminant degradation was observed on g-C3N4, likely due to differences in reactive oxygen species production and/or contaminant-photocatalyst interfacial interactions on different g-C3N4 samples. Moreover, g-C3N4 is a robust photocatalyst for contaminant degradation in raw natural water and (partially) treated water and wastewater. In summary, DFT simulations are a viable tool to predict photocatalyst properties and oxidation performance for contaminant removal, and they guide the rational design, fabrication, and implementation of visible-light-responsive g-C3N4 for efficient, robust, and sustainable water treatment.