Electron Transport Capability Research Articles

3D monolithic composites TiO2/HKUST-1/RGO@melamine foam with improved surface mass transfer for efficient photocatalytic degradation of toluene gas

Currently, photocatalytic technology mostly uses powdered TiO2 catalysts, which are not conducive to recycling, limit the contact between volatile organic compounds (VOCs) and the photocatalyst, and result in lower mass transfer efficiency in gas-solid reactions. Meanwhile, TiO2 catalysts including the electrospun TiO2 nanofibers with hydrophilic surfaces are not favorable for the infiltration and adsorption of non-polar VOCs. To solve these problems, in this work, the monolithic composites TiO2/HKUST-1/RGO@melamine foam (named MRTH) with improved surface mass transfer composed of metal-organic framework (HKUST-1), graphene oxide (GO) and electrospun TiO2 nanofibers was designed. The metal-organic framework HKUST-1 plays a role in promoting the adsorption of toluene, while the reduced graphene oxide (RGO) facilitates the infiltration of non-polar molecules on the surface of the composite and has better electron transport capability. A type II heterojunction between the electrospun TiO2 nanofibers and HKUST-1 formed in the monolithic composites suppresses the recombination of electron-hole pairs and extends their lifespan. Comparing with the bare electrospun TiO2 nanofibers, the MRTH foam composites exhibit a wider light absorption range, hydrophilic and oleophobic properties and a higher separation efficiency of photogenerated carriers. In 90 min of dark adsorption, the removal rate of toluene over MRTH-8 was 52.32 %, while under irradiation by xenon lamp for 150 min, the removal rate over MRTH-8 reached 90.15 %. The amount of monolithic foam composites can also be easily adjusted in the reactor to achieve the best possible removal of the contaminant. The prepared composite materials have been characterized in detail, and the possible mechanisms have also been discussed. The foam composites prepared in this work have high catalytic activity and gas-solid reaction mass transfer efficiency, so they have wide practical application prospects in the field of VOCs abatement.

The synergistic effect of POM-π interaction and solid phase amidation on the visible light photocatalytic of g–C3N4–based photocatalyst

Due to the unique ability of Keggin-type polyoxometalate (POM) to remain stable when accepting electrons to form mixed valence POM, organic-POM hybrid materials can complete multi-electron transfer while maintaining structural stability. The organic-POM hybrids photocatalysts prepared using organic materials and POM as raw materials have been developed to form new energy bands and crystal structures. This not only enhances their quantum efficiency and but also expands their visible light response range. Nevertheless, organic-POM hybrids, featuring organic amines as ligands, are prone to photoetching, impeding g-C3N4's progress in this area. In this paper, the amino group of g-C3N4 was converted into imide ring by solid phase amidation method, which overcame this obstacle and converted g-C3N4 into g-C3N4 based polyimide (CNPI) with enhanced photoelectric properties. XRD, IR spectrum, and XPS data indicate that CNPI is more tightly integrated with potassium phosphotungstate (KPW) than g-C3N4, demonstrating superior electron transport capabilities and potentiated POM-π interactions. In terms of photocatalytic efficacy, CNPI/KPW-30 % exhibits an impressive degradation rate constant of 0.5458 h−1 for imidacloprid, attributed to its compact microstructure and superior charge transfer capability. While maintaining good photocatalytic stability, the mineralization rate of CNPI/KPW-30 % to imidacloprid was 55.25 %. In addition, h+ and ·O2− were identified as active species through trapping agent experiments, and the degradation pathway was advanced by ESR technology analysis.

Ternary organic bulk-heterojunction strategy enables efficient light utilization for perovskite solar cells

Extending the photoresponse into the near-infrared region (NIR) is an urgent research topic in perovskite solar cells. A ternary bulk heterojunction (BHJ) layer composited with PC61BM, D18-Cl and Y6 was deposited onto the perovskite to broaden light absorption. The ternary BHJ layer can absorb low-energy photons in the NIR region (800–920 nm) and generate excitons. Subsequently, these excitons dissociate into free electrons and holes at the donor-acceptor interface, thus extending the device's photo response up to 920 nm. Moreover, due to the good electron transport capabilities of the acceptors Y6 and PC61BM in the BHJ film, the BHJ layer also acts as the electron transport layer in the inverted PSC device. The inverted P–I–N device based on perovskite/BHJ achieved an external quantum efficiency (EQE) up to 30% in the near-infrared range. Compared to control PSCs, the short-circuit current (JSC) increased from 21.64 to 24.35 mA cm−2, resulting in a high PCE of 19.88%. Additionally, the high hydrophobic surface of the ternary layer contributes to the good long-term stability of the device. The results demonstrate that the ternary organic bulk heterojunction is an effective strategy for achieving efficient light utilization in the near-infrared region and enhancing power conversion efficiency in perovskite solar cells.

Electrochemical impedance spectroscopy analysis of dye-sensitized solar cells composed of electrospun composite photoanodes: A comparative study of natural and synthetic sensitizers

In this study, a transmission line model is applied to the electrochemical impedance spectroscopy (EIS) data of the fabricated dye-sensitized solar cells (DSSCs) to evaluate the charge transfer mechanism through the cells. Natural dye from black plum (Syzygium cumini) fruit was used as a cell sensitizer (SC-DSSC) and compared its photovoltaic and electron transport capabilities to those of a cell using a synthetic sensitizer (N719-DSSC). TiO2/ZnO electrospun composite nanofibers were used as the semiconductor layer of the photoanode to enhance electron transfer. The EIS analysis revealed the role of electron resistances through shant, interfaces, and electrolyte solution by measuring the electron transfer kinetic parameters of each element. Based on the results, the SC-DSSC and N719-DSSC are appropriate photovoltaic cells because their ratios of effective electron diffusion length to photoanode thickness are 12.5 and 2.8, respectively. The EIS analysis showed that the electrospun composite nanofiber coated on the photoanode reduces the semiconductor layer's electrical resistance to the cell's total resistance. The extracted natural dye also boosted electron lifetime to 3.68 ms and diffusion coefficient to 54.3×10−6 m2/s while minimizing back-electron recombination at the semiconductor-electrolyte interface. Moreover, the semiconductor-electrolyte interface resistance is over 85% of the overall resistance for both DSSCs and controls electron transport through the cells, which is due to the dye-semiconductor binding intensity. Based on the photovoltaic data, the SC-DSSC cell efficiency was lower than N719-DSSC which is attributed to its higher electron transfer rate-controlling element. Thus, enhancing dye-semiconductor interactions will decrease the rate-controlling impedance and enhance cell performance.

New Electron‐Transporting Materials Based on Pyrimidine and Thiazolopyridine Moieties for High‐Efficiency Organic Light‐Emitting Diodes

Using the pyrimidine moiety with electron‐accepting capability and the thiazolopyridine moiety, commonly used as a moiety with an electron‐withdrawing group in organic semiconductors, for the first time 2‐(3‐(4,6‐di(phenanthren‐9‐yl)pyrimidin‐2‐yl)phenyl)thiazolo[5,4‐b]pyridine (DPPTP) is designed and synthesized to enhance electron transport capabilities compared to the conventional electron‐transporting layer, tris(8‐hydroxyquinoline)aluminum (Alq3). The photoluminescence maxima in solution and film states are observed at 391 and 410 nm, respectively. Although the photoluminescence quantum yield is relatively low at 2% in the solution state, it increases to 28% in the film state. The measured electron mobility values from the fabricated device range from 1.46 × 10−5 to 2.0 × 10−5 cm2 V−1 s−1, ≈5.7 times faster than the electron mobility of Alq3. In a fluorescent blue device utilizing the newly synthesized DPPTP as the electron‐transporting layer, the current efficiency is 4.36 cd A−1, and the external quantum efficiency is 3.76%, representing a 1.3‐fold improvement in efficiency compared to Alq3 devices.

Phosphorus doped magnetic biochar activated PMS for effective degradation of pesticide in water: Targeted regulation of interfacial charge transfer by phosphorus doping

In this study, the incorporation of phosphorus (P) atoms into magnetic biochar was strategically achieved, and the preparation conditions of the composites were optimized by adjusting the pyrolysis temperature and iron doping. The resulting P-doped magnetic biochar (Fe2P@BC-700) exhibited remarkable catalytic activity towards peroxymonosulfate (PMS), rendering it highly effective for the degradation of common organic pesticides, such as 2-Methyl-4-chlorophenoxyacetic acid (MCPA), in aqueous environments. Among them, the apparent rate constant in the oxidation stage was 6.42 times as large as that of magnetic biochar (Fe2BC-700). This was attributed to the fact that the introduced P species tuned the surface electronic configuration of the pristine carbon layer with excellent electron storage and transport capabilities, and the Fe-O-P bonds in the composites acted as electron transport bridges to promote iron cycling in the magnetic nanoparticles during catalysis. The elimination of MCPA in the constructed adsorption enrichment-oxidative degradation system (Fe2P@BC-700/PMS) was achieved through a non-radical pathway dominated by singlet oxygen (1O2) and electron transfer process (ETP). It also ensured broad pH adaptability, environmental stability and repeatability. Density-functional theory calculated that ROS tended to attack the C-Cl branched chain in MCPA and the degradation products showed a tendency of toxicity reduction. This study provided new ideas for the design of market-oriented functional biochar catalysts.

Facilitating Electron Transport in Perovskite Solar Cells Through Tailored SnO2 Film Composition

The ratio of Sn2+ to Sn4+ plays an essential role in influencing the characteristics of SnO2 film, which is commonly used in the normal structure of perovskite solar cells (PSCs). It is identified that different sequences of addition lead to varying concentrations of Sn2+ and Sn4+ within the SnO2 film. Through this strategic approach, an enhanced SnO2 film with improved electron transport capabilities, a smoother surface texture, and more suitable energy levels are successfully engineered. Consequently, the efficiency of PSCs has seen a notable increase from 22.58% for the control device to 24.16% for the target PSC. Furthermore, PSCs utilizing the optimized SnO2 have demonstrated superior long‐term environmental stability when compared to the control devices. Specifically, PSCs incorporating optimized SnO2 expose to approximately 30% humidity in ambient air for 41 days without encapsulation retain 87% of their initial efficiency. In contrast, the control devices under the same conditions only maintain 77% of their original value.

Cu2ZnSnS4/N-MWCNTs hybrid systems as counter electrode substitutes for platinum in dye-sensitized solar cells

Copper zinc tin sulfide, Cu2ZnSnS4 (CZTS) is being considered a viable option for a counter electrode due to its abundance, cost-effectiveness, catalytic activity, and other advantageous properties. However, CZTS has low electron transport capabilities, a shortcoming that can be addressed by combining it with high electron mobility carbon nanomaterials. Nitrogen-doped multi-walled carbon nanotubes (N-MWCNTs) exhibit higher electron conductivities than their pristine counterparts. This improvement is attributed to the disruption of the sp2-hybridized carbon arrangement, as some of the carbon atoms are replaced by nitrogen atoms. In this study, a counter electrode composed of a 70% CZTS and 30% N-MWCNTs mixture produced a higher electrochemical current density compared to the individual materials. This suggests that it is more electrocatalytic than CZTS and N-MWCNTs alone, ultimately leading to the highest power conversion efficiency of 6.52%.Graphical abstract

“Graphene Bubble Bridging” Enabled Flexible Multifunctional Carbon Fiber Membrane Toward K+ Storage Devices

AbstractWidespread integration of carbon‐based membranes into prevailing fields like energy storage and material engineering is thwarted by a lack of functionality, customization, and compatibility, making the development of such carbon‐based membranes urgency yet challenging. Herein, a “graphene bubble bridging” strategy is adopted to fabricate the multifunctional carbon fiber membrane, in which graphene bubbles with optimized assembling not only endow the carbon fiber with superior flexibility and integrity by embedded bridging function, but also enhance the fast electron transport capability and electrolyte wettability. Few‐layer MoSSe nanosheets with expanded interlayer spacing as a typical energy storage material contribute to plentiful ion intercalation/deintercalation that can be well buffered within the robust fibers. The interlaced carbon fibers enable a self‐supporting framework that ensures good conductivity and mechanical stability as well. Such functional, customized, and compatible membranes with synergies can boost the attributes of advanced K+ storage devices, such as flexible K‐ion capacitors and K‐based dual‐ion batteries. This work can afford new insights for designing flexible electrode in the energy storage field, as well as various types of conformations that can bring more opportunities on developing flexible functional membranes for other fields (e.g., catalysts, electromagnetic shielding).

Enhancing the stability and efficiency of carbon-based perovskite solar cell performance with ZrO2-decorated rGO nanosheets in a mesoporous TiO2 electron-transport layer.

Improving the role of electron-transport layers (ETLs) in carbon-based perovskite solar cells (CPSCs) is a promising method to increase their photovoltaic efficiency. Herein, we employed rGO sheets decorated with ZrO2 nanoparticles to increase the electron transport capability of mesoporous TiO2 ETLs. We found that the rGO/ZrO2 dopant enhanced the conductivity of the ETL, reducing the charge-transfer resistance at the ETL/perovskite interface and reducing charge recombination in the corresponding CPSCs. Notably, this dopant did not effectively change the transparency of ETLs, while increasing the light-harvesting ability of their own top perovskite layer by improving the crystallinity of the perovskite layer. The rGO/ZrO2-containing ETLs produced a champion efficiency of 15.21%, while devices with a net ETL recorded a maximum efficiency of 11.88%. In addition, the modified devices showed a higher stability behavior against ambient air than the net devices, which was linked to the passivated grain boundaries of the modified perovskite layers along with the improved hydrophobicity.

Self-assembled molecular network with waterwheel-like architecture: experimental and theoretical evaluation toward electron transport capabilities for optoelectronic devices.

In recent times, self-assembled electron transport materials for optoelectronic devices, both solar cells and organic light-emitting diodes (OLEDs), have been gaining much interest as they help in fabricating high-efficiency devices. However, designing organic small molecular materials with star-shaped self-assembled networks is a challenge. To achieve this sort of target, we chose triazine and benzene-1,3,5-tricarbonyl cores for developing such architecture, and we developed four molecular systems, vizTCpCN, TCmCN, TmCN, and TpCN. Successful isolation of single crystals followed by structural analysis of TmCN revealed interesting molecular arrangements in the solid state resulting in the formation of a waterwheel type architecture with an extended network bearing characteristic voids. Theoretical calculations was carried out to check their electron transportability. The natural transition orbital calculation helped in understanding the locally excited and charge transfer excited states. The low electron reorganization energies of these molecules indicated that these materials may have potential to be used in electron transport layers of optoelectronic devices, particularly in OLEDs. Moreover, the assembled networks have a relatively wide surface area and linked structures, which are advantageous for the conduction of carriers with poor electron recombination inside the ETL, and these may offer a straightforward channel for electron conduction to the emissive layer. Finally, the fabricated electron-only device indicated that the synthesized materials may be used as ETMs in the electron transport layer of optoelectronic devices.

Controlled synthesis of 2D-2D conductive metal-organic framework/g-C3N4 heterojunctions for efficient photocatalytic hydrogen evolution.

Designing photocatalysts with efficient charge separation and electron transport capabilities to achieve efficient visible-driven hydrogen production remains a challenge. Herein, 2D-2D conductive metal-organic framework/g-C3N4 heterojunctions were successfully prepared by an in situ assembly. Compared to pristine g-C3N4, the ratio-optimized Ni-CAT-1/g-C3N4 exhibits approximately 3.6 times higher visible-light H2 production activity, reaching 14 mmol g-1. Through investigations using time-resolved photoluminescence, surface photovoltage, and wavelength-dependent photocurrent action spectroscopies, it is determined that the improved photocatalytic performance is attributed to enhanced charge transfer and separation, specifically the efficient transfer of excited high-energy-level electrons from g-C3N4 to Ni-CAT in the heterojunctions. Furthermore, the high electrical conductivity of Ni-CAT enables rapid electron transport, contributing to the overall enhanced performance. This work provides a feasible strategy to construct efficient dimension-matched g-C3N4-based heterojunction photocatalysts with high-efficiency charge separation for solar-driven H2 production.

Solution processed PANI-rGO-SiO2 nanocomposite with inflated electron injection and transport capabilities as ETL for OLED applications

PANI-rGO-SiO2 nanocomposite as an ETL with varying concentrations of SiO2 was synthesized via oxidative in-situ polymerization process. Their structural and optical properties were investigated by XRD, FESEM, FTIR, Photoluminescence and UV–Vis. Spectroscopy. The PANI depicted a nanofiber-like structure with uniform distribution. The optical band gap of the optimized PGS1 nanocomposite was estimated ∼ 3.01 eV in the visible region of electromagnetic spectrum. TGA results revealed lesser weight loss ∼ 12 % in case of PGS1 nanocomposite than PANI. The light absorption was found at 481 nm in blue region due to charge transfer of SiO2 and PANI-rGO matrix. The current density of PGS1 nanocomposite was observed 76 % greater than pristine PANI using J-V characteristics which showed greater capacities to transfer electron from cathode into emissive layer. These results elucidate that the optimized PGS1 nanocomposite is a compatible candidate for an electron transport layer (ETL) in OLED applications.

Cation Defect-Engineered Boost Fast Kinetics of Two-Dimensional Topological Bi2 Se3 Cathode for High-Performance Aqueous Zn-Ion Batteries.

The challenge with aqueous zinc-ion batteries (ZIBs) lies in finding suitable cathode materials that can provide high capacity and fast kinetics. Herein, two-dimensional topological Bi2 Se3 with acceptable Bi-vacancies for ZIBs cathode (Cu-Bi2-x Se3 ) is constructed through one-step hydrothermal process accompanied by Cu heteroatom introduction. The cation-deficient Cu-Bi2-x Se3 nanosheets (≈4nm) bring improved conductivity from large surface topological metal states contribution and enhanced bulk conductivity. Besides, the increased adsorption energy and reduced Zn2+ migration barrier demonstrated by density-functional theory (DFT) calculations illustrate the decreased Coulombic ion-lattice repulsion of Cu-Bi2-x Se3 . Therefore, Cu-Bi2-x Se3 exhibits both enhanced ion and electron transport capability, leading to more carrier reversible insertion proved by in situ synchrotron X-ray diffraction (SXRD). These features endow Cu-Bi2-x Se3 with sufficient specific capacity (320mAhg-1 at 0.1Ag-1 ), high-rate performance (97mAhg-1 at 10Ag-1 ), and reliable cycling stability (70mAhg-1 at 10Ag-1 after 4000 cycles). Furthermore, quasi-solid-state fiber-shaped ZIBs employing the Cu-Bi2-x Se3 cathode demonstrate respectable performance and superior flexibility even under high mass loading. This work implements a conceptually innovative strategy represented by cation defect design in topological insulator cathode for achieving high-performance battery electrochemistry.

Supramolecularly engineered S-scheme SubPc-Br/MoS2 photocatalyst nanosheets for enhanced photocatalytic degradation of antibiotics

Developing a simple, low-cost, high-yield, and controllable strategy for preparing various functionalized MoS2-based composite materials remains a challenge. This study innovatively utilizes boron subphthalocyanine bromide (SubPc-Br) as a photosensitizer, which self-assembles on MoS2 via intermolecular π-π stacking, creating a SubPc-Br/MoS2 organic–inorganic semiconductor system. This addresses a research gap, employing subphthalocyanines as MoS2 sensitizers. The SubPc-Br/MoS2 heterojunction exhibited excellent photocatalytic activity for the degradation of antibiotics in water under solar irradiation. The rate constants for the photocatalytic degradation of CTC and CIP by SubPc-Br/MoS2 were 4.66 and 5.93 times higher than those of pristine MoS2, respectively. The significant improvement in photocatalytic performance is attributed to the efficient charge separation and transfer induced by the unique S-Scheme charge transfer mechanism, which has been verified by different theoretical and experimental results. We demonstrate that the photochemical activity of O2 molecules adsorbed on MoS2(100) is site-sensitive, with O2 preferentially adsorbing on the Mid-site location with higher electron transport capability. This study provides a new perspective for enhancing photocatalytic performance by constructing an artificial photosynthetic system with an S-scheme heterojunction.

Effects of Microplastics on Soil Carbon Mineralization: The Crucial Role of Oxygen Dynamics and Electron Transfer.

Although our understanding of the effects of microplastics on the dynamics of soil organic matter (SOM) has considerably advanced in recent years, the fundamental mechanisms remain unclear. In this study, we examine the effects of polyethylene and poly(lactic acid) microplastics on SOM processes via mineralization incubation. Accordingly, we evaluated the changes in carbon dioxide (CO2) and methane (CH4) production. An O2 planar optical sensor was used to detect the temporal behavior of dissolved O2 during incubation to determine the microscale oxygen heterogeneity caused by microplastics. Additionally, the changes in soil dissolved organic matter (DOM) were evaluated using a combination of spectroscopic approaches and ultrahigh-resolution mass spectrometry. Microplastics increased cumulative CO2 emissions by 160-613%, whereas CH4 emissions dropped by 45-503%, which may be attributed to the oxygenated porous habitats surrounding microplastics. Conventional and biodegradable microplastics changed the quantities of soil dissolved organic carbon. In the microplastic treatments, DOM with more polar groups was detected, suggesting a higher level of electron transport. In addition, there was a positive correlation between the carbon concentration, electron-donating ability, and CO2 emission. These findings suggest that microplastics may facilitate the mineralization of SOM by modifying O2 microenvironments, DOM concentration, and DOM electron transport capability. Accordingly, this study provides new insights into the impact of microplastics on soil carbon dynamics.

Interface Engineering and Boron Modification of Pd-B/Pd Hetero-Metallene Synergistically Accelerate Oxygen Reduction Catalysis.

2D metallene possess high surface area and excellent electron transport capability, thus enabling efficient application in oxygen reduction reaction (ORR). However, the interface regulation and electronic structure optimization of metallene are still great challenges. Herein, Pd-B/Pd hetero-metallene is constructed by interface engineering and B modification strategies for efficient electrocatalytic ORR. The 2D configuration of Pd-B/Pd hetero-metallene exposes a large number of surface atoms and unsaturated defect sites, thus providing abundant catalytic active sites and exhibiting high electron mobility. More importantly, interface engineering and B modification synergistically optimizing the electronic configuration of the metallene system. This work not only provides an effective strategy for the rational regulation of the electronic configuration of metallene, but also offers a reference for the construction of efficient ORR catalysts.

In-site grown carbon nanotubes connecting Fe/Cu-N-C polyhedrons as robust electrocatalysts for Zn-air batteries

Fe-N-C catalysts are considered to be the most promising non-precious metal based catalysts for oxygen reduction reactions (ORRs), but the low active site density and the insufficient electron transport capability have seriously impeded their applications in fuel cells and metal-air batteries. Herein, we demonstrate polyhedral Fe/Cu-N-C particles chained by in-site grown carbon nanotubes (CNTs) serving as robust electrocatalysts for Zn-air battery (ZAB) applications. Benefiting from highly exposed polyhedral active sites and FeCu induced in-site grown CNT channels as well as Fe, Cu bimetallic synergistic optimization of adsorption/desorption energy, the engineered Fe/Cu-N-C electrocatalyst exhibits outstanding oxygen reduction performance. The ultrahigh activity of the Fe/Cu-Nx catalytic centers is attributed to not only the high content of pyridinic and graphitic N, but also the enhanced electron density around Fe atom center. Both primary and rechargeable ZABs are assembled and tested. The results show that the Fe/Cu-N-C based ZABs are far superior to the commercial Pt/C based ZABs regarding peak power density, specific capacity, energy density and cycling stability.

Ultrafast synthesis of 3D porous flash graphene and its adsorption properties

3D hierarchical porous graphene (3D HPG) has recently captured significant attention due to its unique porosities, excellent electron transport capability, and multifunctionality. However, given that the traditional preparation method of 3D HPG is time-consuming, energy-consuming and seriously polluting, which seriously block its wide application. This study leveraged the capabilities of flash Joule heating (FJH) to ultrafast synthesize 3D porous flash graphene (3D PFG) with good dispersion and adsorption properties from bituminous coal (BC) within 21 s. The thermal shock generated by carbonate pyrolysis and the thermal expansion generated by Joule heating were used to produce the stable porous structure. Moreover, the specific surface area of 3D PFG was as high as 504 m2g−1, and displayed the characteristics of hierarchical porous structure of micropores, mesopores and macropores. The porous structure changes of 3D PFG synthesized by FJH under different carbonate ratios and different flash voltages were investigated, and the controllable synthesis conditions of hierarchical pore structures during FJH were obtained accordingly. As the experimental and simulation results show, the 3D PFG displays good dispersibility and good adsorption performance as adsorbent for methylene blue and methyl orange. This environmentally friendly synthetic process of FJH not only simplifies the preparation process of 3D HPG but also provides a valuable way for the high value-added utilization of coal.

Efficient removal of chloroform from groundwater using activated percarbonate by cellulose nanofiber-supported Fe/Cu nanocomposites

Chloroform (CF) is a recalcitrant halogenated methane (HM) that has received widespread attention due to its frequent detection in groundwater and its potential carcinogenic risk. In this study, TEMPO-oxidized cellulose nanofiber-supported iron/copper bimetallic nanoparticles (TOCNF-Fe/Cu), a novel composite catalyst, was synthesized to activate sodium percarbonate (SPC) for the removal of CF from groundwater. The results showed that over 96.3% of CF could be removed in a neutral reaction medium (pH 6.5–9) within 180 min using 0.66 g L−1 of TOCNF (0.32)-Fe/Cu (1) and 1 mM of SPC, which outperforms typical advanced oxidation processes. The reaction mechanism of the TOCNF-Fe/Cu-SPC system for the CF removal was elucidated. As demonstrated through electron paramagnetic resonance and quenching experiments, the TOCNF-Fe/Cu-SPC system was found to include •OH and O2•−, where the latter played a dominant role in the CF removal. DFT calculations indicated that TOCNF improved the electron transport capability of Fe/Cu and reduced the transition state energy. The Fe species on the surface of TOCNF-Fe/Cu were identified as the primary active sites for SPC activation, whereas the Cu species were beneficial to the regeneration of the Fe species. Additionally, TOCNF-Fe/Cu was found to have good recyclability and stability. The feasibility of the TOCNF-Fe/Cu-SPC system was further confirmed by applying it for the efficient removal of composite HMs from actually contaminated groundwater. Overall, the TOCNF-Fe/Cu-SPC system is an attractive candidate for the treatment of HM-contaminated groundwater.