3D printing has gained great attention in electrochemical CO2 reduction (CO2RR), however, its use in constructing self-supported catalytic electrodes with well-dispersed coordination active sites is still underdeveloped. In this study, a catalytic electrode with CoNX coordination structures (3D-CE-CoNX) was successfully fabricated using 3D printing for syngas production via CO2RR. The CO2RR reaction was conducted in a H-type electrolyzer, which was equipped with a conventional three-electrode system. Electrochemical tests show that 3D-CE-CoNX, carbonized at 700 degrees C, exhibits good CO2 reduction activity within the potential range of -0.6 V to -1.0 V, producing syngas with a H2:CO ratio ranging from 0.53 to 1.79, which is tunable mainly by the applied potential. At -0.7 V, the current density for CO (JCO) is -0.19 mA cm- 2, while for H2 (JH2)is -0.14 mA cm- 2. After 24 h of continuous electrolysis, 3D-CE-CoNX maintains 91.5% of its initial CO faradaic efficiency (FECO). Furthermore, Xray absorption fine structure (XAFS) characterization confirms the successful incorporation of CoNX sites, validating the electrode's effectiveness. This study highlights the unique advantages of 3D printing in catalytic electrode construction and provides a feasible pathway for obtaining high-performance catalytic electrodes for future energy conversion applications.
The development of catalytic electrode by 3D printing technology has become a hot spot. In this study, a catalytic electrode for CO2 reduction reaction (CO2RR) (named DIW-FePc-CE) was fabricated using direct ink writing (DIW) 3D printing technology, with iron phthalocyanine (FePc) was loaded at varying concentrations via an impregnation method. The results showed that, CO was the main product and H2 was the only by-product (small amounts) on as-prepared DIW-FePc-CE. Notably, the optimal DIW-FePc-CE (carbonized at 950 degrees C and soaking with 8 g L- 1 FePc) showed high selectivity for electroreduction conversion of CO2 into CO with a high Faraday efficiency (FECO) of 63.3 %. And the FECO was basically stabilized for 8 h of continuous electrolysis. This study fabricated catalytic electrodes for CO2RR, offering a valuable reference for the development of other advanced catalytic electrodes using DIW technology.
Self-fueling and energy-blocking played important roles in enhancing the antitumor efficacy of reactive oxygen species (ROS) therapy. Here, a novel nanozyme (CuS@Pd/DHA@ZnO2) was constructed by loading dihydroartemisinin (DHA) and coating palladium nanoparticles (PdNPs) and zinc peroxide (ZnO2) on the hollow copper sulfide (CuS), and the enhanced antitumor efficacy was arrived through self-fueling and energy-blocking strategies. In the acidic tumor microenvironment, the ZnO2 decomposed to produce H2O2 and Zn2+, which effectively improved the hydroxyl radicals generation performance of PdNPs and Cu+, and induced the superoxide anion and C-free radicals generation performances by Zn2+ and Cu2+/DHA, resulting in the accumulation of ROS. Moreover, Zn2+ and ROS storm disrupted synergistically the mitochondrial function, and caused the energy-blocking. Ultimately, by combining the self-fueling and energy-blocking strategies, the tumor growth was almost completely inhibited, demonstrating the excellent antitumor efficacy of CuS@Pd/DHA@ZnO2 nanozyme.
Designing economical Fe-N-C catalysts capable of substituting platinum-based counterparts in oxygen reduction reaction (ORR) continues to be a pivotal obstacle for driving progress in sustainable energy systems. Herein, Pdoping and two-dimensional MXene introducing were jointed to construct an enhanced version of the Fe-N-C system, which has a flower-like structure naming as Fe-NP-C/MX. By studying the ratios and carbonized temperatures of the precursors (triphenylphosphine, Fe(NO3)2 and MXene), the optimal fixed at 2:1 (Fe(NO3)2 / triphenylphosphine) under carbonized at 900 degrees C. It showed good ORR performance with the E1/2 of 0.88 V, which is better than that of Pt/C (E1/2 = 0.85 V). Importantly, when assembled into zinc-air batteries (ZABs) devices, a peak power density of 177.2 mW cm-2 was achieved, in which only a decay rate of 6.41% was detected during a 48,000 s continuous test (better than Pt/C (18.13%)). This work offers a good reference for developing other enhanced Fe-N-C system with joint enhancement strategy.
The CO2 in industrial flue gas is an attractive renewable carbon source for electrocatalytic conversion. Herein, a silver-doped copper selenide catalyst (Ag-CuxSe/C) was developed for efficient CO2 electroreduction under both high-purity CO2 (> 99.9%) and simulated flue gas (15.0% CO2). Notably, Ag incorporation modulates the electronic structure of the Cu-Se matrix and improves the catalytic selectivity and stability toward ethanol (EtOH) production. At -0.7 V, the Ag-CuxSe/C catalyst achieves a faradaic efficiency for EtOH (FEEtOH) of 64.20% under pure CO2, and 49.38% under flue gas conditions. Moreover, it maintains high EtOH selectivity (50.35%) over 48 h of continuous operation in flue gas, demonstrating good durability. This work would provide a good reference for the sustainable development of CO2 capture and conversion from flue gas in future.
Electrochemical CO2 reduction to multicarbon (C2+) products offers a viable pathway for renewable energy storage and carbon-neutral fuel synthesis, yet achieving high current density and selectivity simultaneously remains challenging due to limited CC coupling efficiency. Here, we report a facile H2O2-assisted anion-exchange strategy to construct CuO nanosheets enriched with grain boundaries and defect sites, enabling efficient CO2-to-C2+ electrosynthesis at ampere-level current densities. The optimized CuO-H2O2 catalyst delivers a C2+ Faradaic efficiency of 81.8% with a partial current density reaching 867 mA cm−2. Operando spectroscopic analysis combined with density functional theory calculations reveals that the defect-rich surface promotes *CO adsorption and induces a locally alkaline microenvironment, which together lower the energy barrier for asymmetric *CO-*CHO coupling. This dual effect enhances CC bond formation kinetics and drives selective C2+ production. These findings establish defect-engineered Cu catalysts as an effective platform for high-rate CO2 electroreduction and provide mechanistic insights into coupling microenvironment regulation with intermediate stabilization for efficient multi‑carbon synthesis.
Three-dimensional (3D) printing offers a versatile and advanced manufacturing approach for the fabrication of catalytic electrodes. In this study, 3D-printed catalytic electrode was prepared, anchored with Cu-based complex ([Cu(phen)2]2+), (3D-CuNC), which is designed for the electrochemical CO2 reduction reaction (CO2RR). The introduction of [Cu(phen)2]2+ provides CO2RR catalytic sites, while the design flexibility of 3D printing endows the 3D-CuNC electrode with customizability, achieving a high Faradaic efficiency (FE) of 87.07 % for CO production, with H2 as the primary byproduct (12.93 %). Furthermore, the 3D-CuNC demonstrated good long-term stability, maintaining a high FE of 86.64 % after 12h of continuous electrolysis. The used 3D printing approach provides a powerful and customizable strategy for the design and fabrication of high-performance CO2RR catalytic electrodes in future.
To improve the CO2 reduction reaction (CO2RR) performance, catalytic electrodes capable of effectively suppressing the competing hydrogen evolution reaction (HER) are crucial. Herein, a Cu-complex catalytic electrode (CuN/B-P+-3DCE) was fabricated via 3D printing, onto which [Cu(phen)2]2+ complex active sites (Cu-N4) were established and BPh4-/PPh4+ ion pairs were further incorporated to effectively suppress the competing HER. Notably, the resulting CuN/B-P+-3DCE electrode achieved a CO Faradaic efficiency of 94.3% at-0.7 V (vs. RHE), along with good long-term operational stability over 12 h. Importantly, 3D printing enables precise structural design while minimizing the environmental impact of electrode fabrication by reducing chemical waste and energy consumption. Meanwhile, ion-pair modulation effectively directs reaction selectivity toward CO production, thereby enhancing energy efficiency and overall reaction sustainability. This work demonstrates a dual green strategy integrating sustainable electrode fabrication and selective catalytic regulation, offering new insights into environmentally benign CO2 electroreduction systems.
Developing efficient platinum group metal-free (PGM-free) electrocatalysts for oxygen reactions is crucial for advancing next-generation renewable energy technologies. Herein, a bifunctional oxygen catalyst of Ironphthalocyanine coupled Nickel-oxide depositing on carbon-peeled MXene (NF/MC3), is proposed as a promising PGM-free alternative. This catalyst exhibits good catalytic performance under alkaline conditions, delivering a half-wave potential (E-1/2) of 0.928 V for the oxygen reduction reaction (ORR) and an oxygen evolution reaction (OER) overpotential (E-i = 10) of 1.731 V. When applied in zinc-air batteries (ZABs), the assembled device achieves a high-power density of 151.8 mW cm(-2) and a current density of 292.0 mA cm(-2), maintaining stable stability over 167 h of continuous charge-discharge cycling. This work provides valuable insights into the design of highly efficient and durable non-precious metal catalysts, paving the way for the development of costeffective, high-performance energy conversion and storage systems.
MXene-based supercapacitors, serving as highly efficient energy storage components, are experiencing increasing utilization in industrial electronics and wearable technologies. These devices integrate exceptional power density, rapid charge-discharge capability, and remarkable cyclic stability, positioning them as pivotal enablers for next-generation autonomous and portable systems. However, their practical deployment is constrained by inherent environmental sensitivity, where issues such as material instability, susceptibility to contamination, and structural degradation significantly impair their electrochemical performance and operational durability under extreme conditions, thereby limiting their potential application scope. Consequently, systematic investigation into their behavior under such demanding circumstances is essential to unlock their full potential for critical fields including aerospace, deep-sea exploration, and biomedical devices. Herein, this review consolidates recent research advances in MXene-based supercapacitors designed for harsh operational environments. It systematically summarizes their performance characteristics and corresponding mitigation strategies under extreme temperatures, variable humidity, dynamic pressures, and other specialized conditions, while providing an in-depth analysis of prevailing application gaps and persistent scientific challenges. Finally, this work outlines prospective development pathways for MXene-based supercapacitors targeting even more severe application scenarios, offering a foundational roadmap to broaden their applicability and accelerate their advancement across multiple domains.
Intrinsic defect-rich carbon is prepared via alkali-assisted pyrolysis of C60. Via Joule heating, this defective carbon yields Pt particles with an ultrafine size of 2.5 nm within seconds. Due to the favorable defect-induced electron transfer, this Pt catalyst shows significantly enhanced activity and stability towards alkaline oxygen reduction.
Developing efficient, synthetically simple ammonium-retention materials for soil ammonium immobilization and nitrogen-loss mitigation remains challenging because competitive soil matrices require accessible binding interfaces, rapid ion transport, and structural robustness. Herein, a carbon dots@Ca-Al layered double hydroxides (CDs@LDHs) hybrid was synthesized via one-pot in situ carbonization for NH4+-N immobilization. Oxygen-rich CDs anchored onto LDHs via C-O-M coordination could generate a mesoporous architecture with strong negative surface polarization (−42.7 mV). Driven by electrostatic attraction and hydrogen bonding, CDs@LDHs were able to achieve an aqueous NH4+-N adsorption capacity of 14.26 mg/g, outperforming commonly-used biochar and zeolite under identical aqueous conditions. In competitive soil environments, a low dosage (0.1 wt%) retained >60% NH4+-N. Furthermore, soil incubation could reduce cumulative NH3 volatilization by >40% and apparent nitrification by >50%, increasing total nitrogen by 8.8%. These superior performances were attributed to chemically integrated interfacial polarization and accessible oxygen-rich sites. Our success would offer a scalable material platform to improve fertilizer-use efficiency and moderate environmental nitrogen loss.
The service reliability of wheelset bearings in railway freight cars is essential for ensuring transportation safety and efficiency. With increasing axle loads and operating speeds, traditional phosphate-treated bearings are increasingly susceptible to fatigue, wear, and corrosion under harsh service conditions. These issues have become critical bottlenecks limiting bearing service life. Diamond-like carbon (DLC) films, as high-performance carbon-based surface coatings, offer a promising technical solution to these challenges given their excellent friction-reducing, wear-resistant, corrosion-resistant, and insulation properties. This review summarizes the service conditions of railway freight car wheelset bearings and focuses on recent research progress in the tribological, fatigue-resistant, corrosion-resistant, and insulation performance of DLC films under such demanding environments. Moreover, leveraging latest advances in DLC film deposition techniques and process optimization, this work explores the prospective applications of DLC coatings. The discussed directions include developing DLC films dedicated to railway bearings, conducting in-depth research on failure mechanisms and life prediction methods, and revealing the synergistic interactions between DLC films and lubricating greases. This study aims to accelerate the industrial application of this technology for China's heavy-haul railway network.
The rational design of low-Pt catalysts to achieve good catalytic performance has always attracted much attention. In this study, a hybrid cathode electrocatalyst composed of a low-Pt high-entropy-alloy (PtPdAuNiCu) coupled with a carbon-peeled-MXene (CpM) support was developed, termed as PtPdAuNiCu/CpM, for the oxygen reduction reaction (ORR). It arises from combining the entropy-stabilized PtPdAuNiCu alloy with a structurally exfoliated CpM support, where the HEA provides electronic structure modulation, while CpM exposes more active terminations and enhances charge-transfer pathways. The PtPdAuNiCu/CpM catalyst exhibits a higher half-wave potential (E1/2) (0.886 V) compared to 20% Pt/C (0.865 V). Moreover, in the chronoamperometry test, the PtPdAuNiCu/CpM catalyst retains 87.1% of its current after 45,000 s, compared to 81.8% of Pt/C. In addition, in the cycling tests, the PtPdAuNiCu/CpM catalyst exhibits a loss of 28 mV in E1/2 after 2500 cycles, which far less than that of Pt/C (75.7 mV after 1000 cycles). Furthermore, the zinc-air battery (ZAB) cathode equipped with the PtPdAuNiCu/CpM catalyst delivers a maximum power output density of 162.8 mW cm-2 and a current density of 270.8 mA cm-2, surpassing that of the Pt/C+RuO2 system (136 mW cm-2 and 226.3 mA cm-2). This study reduces Pt usage through a coupled HEA-MXene design and offers a good reference for developing other advanced, low-cost electrocatalysts for energy storage applications.
Designing good p/n heterojunctions is of great interest in the pursuit of efficient multi‑carbon product generation through CO2 reduction reaction (CO2RR). Herein, a Co-doped CuSe/Cu2Se p/n-type heterostructure (p/n-CuSe/Cu2Se-Co) was fabricated, which induces interfacial electronic reconstruction and a strengthened built-in electric field, thereby facilitating charge transfer and enhancing the surface coverage/retention of *CO on Cu-related ensembles, ultimately promoting C-C coupling toward ethanol. Notably, as-prepared p/n-CuSe/Cu2Se-Co (10.0%) exhibits an ethanol Faradaic efficiency (FEC2H5OH) of 73.0 ± 1.1% and an ethanol partial current density (jC2H5OH) of -0.496 ± 0.005 mA cm-2 in a flow cell at -0.6 V. Additionally, in simulating flue gas condition, it can output 61.2 ± 1.2% of FEC2H5OH and -0.861 ± 0.003 mA cm-2 of jC2H5OH at -0.6 V. This work would provide a feasible reference of advanced p/n-type heterojunction design, promoting the conversion of CO2-to-ethanol electroconversion.
Electrochemical reduction of carbon dioxide (CO2RR) offers a sustainable pathway for producing fuels and chemicals, yet it is hindered by slow reaction kinetics and a broad spectrum of products. Here, we present a strategy that accelerates CO2RR kinetics by modifying oxide-derived copper (OD-Cu) catalysts with an imidazolium-based ionic liquid (IL), specifically, [Bmim]OH, following the "Solid Catalyst with Ionic Liquid Layer" (SCILL) concept. The modification significantly enhances performance, boosting the overall reduction current density from 75 to 353 mA cm- 2 at -0.9 V vs. RHE. It results in a 3.3-fold increase in the partial current density for C2+ products (110 mA cm- 2) while maintaining high faradaic efficiency. In situ spectroscopy and theoretical calculations suggest that the [Bmim]+ cations facilitate CO2 activation of CO2 via hydrogen bonding interactions, thereby accelerating the rate-determining formation of CO2 center dot- radicals. This study decouples the role of IL cations from anions in CO2RR and uncovers their mechanistic function in stabilizing key intermediates. These insights provide a foundation for rational interfacial engineering strategies to advance sustainable electrochemical conversion.
The innovation of highly efficient without platinum group metals electrocatalysts for the oxygen reduction reaction (ORR) is of critical significance. In pursuit of enhanced ORR performance, in this study, the Fe-N-C framework was rationally engineered by incorporating lanthanum to enrich active sites, while simultaneously integrating conductive MXene to construct rapid electron-transfer pathways. As-prepared FeLa-NC/MXene catalyst exhibits good ORR performance (Eonset = 1.007 V, E1/2 = 0.871 V), and the fabricated zinc-air batteries deliver a the highest power density reaching 163.6 mW cm-2 and maintain durable charge-discharge operation for 167 h. This study would provide some valuable insights into the rational design of advanced M-N-C systems for energy devices in future.
Exploiting its exceptional structural tunability and digital manufacturing capability, 3D printing emerges as a transformative technique for the rational design and scalable fabrication of catalytic electrodes tailored for advanced electrochemical energy systems. In this study, hierarchically porous, self-supporting carbon electrodes were fabricated via 3D printing technique in combination with the sequential conformal carbonization. An optimized polymerizable ionic liquid-based ink was employed to produce a 3D printed polymer gel, which was subsequently functionalized with B-containing species. The as-prepared gel was then pyrolyzed to yield B/N-co-doped carbon electrodes with a high surface area possessing micropores, mesopores and macropores. The metal-free cathode demonstrated good performance in electrocatalytic CO2 reduction, producing syngas with tunable H2/CO ratios ranging from 0.37 to 2.6, thereby catering to diverse application requirements. This study naturally integrates 3D printing with ionic-liquid chemistry to fabricate customizable metal-free carbon electrodes for efficient CO2-to-syngas conversion, offering a Power-to-X route to store intermittent renewable electricity as chemical energy and to deliver tunable H2/CO syngas suitable for downstream fuel and chemical synthesis.
Developing high-performance, low-cost bifunctional oxygen electrocatalysts for the oxygen reduction and evolution reactions (ORR/OER) is critical for advancing rechargeable zinc-air batteries (ZABs). Conventional Fe-N-C single-atom catalysts exhibit promising ORR activity but still need further kinetic optimization, alongside intrinsically inadequate OER performance, limited durability, and severe metal aggregation during pyrolysis. Herein, by integrating in-situ bimetallic co-assembly within a ZIF precursor with molten-NaCl assisted pyrolysis, we synthesize an Fe and Cu co-decorated N-doped hierarchically porous carbon catalyst (FeCu-NHPC). This integrated strategy simultaneously constructs abundant atomically dispersed Fe-N4 and Cu-N4 sites along with minor Fe/Cu nanoparticles, while engineering a hierarchical pore architecture featuring a large surface area (1592.47 m2 g−1) to enhance active-site accessibility and mass transport. Spectroscopic and electrochemical characterizations reveal observable Fe-Cu electronic interactions, identifying Fe-N4 as the dominant ORR active sites and Cu-N4 as key electronic modulators. Consequently, FeCu-NHPC delivers outstanding bifunctional activity with an ORR half-wave potential of 0.90 V and an OER potential of 1.54 V at 10 mA cm−2. Moreover, the extremely low H2O2 yield (∼0.01%) during ORR effectively suppresses Fenton side reactions, while the partially graphitized carbon framework and a small amount of interwoven carbon nanotubes, both originating from Fe species catalysis, collectively ensure outstanding long-term stability. When assembled into ZABs, it achieves an open-circuit voltage of 1.51 V, a peak power density of 171.0 mW cm−2, and exceptional cycling stability over 600 h. This work provides a rational design strategy integrating bimetallic synergy and pore engineering toward high-performance bifunctional electrocatalysts.