Noble metal-based intermetallic compounds (IMCs) with ordered atomic arrangements exhibit remarkable electrocatalytic activity owing to their unique crystal and electronic structures. During the past years, great advance has been made in the development of noble metal-based IMCs. Recently, Lu and coworkers reported ultrathin “amorphous/intermetallic” (A/IMC) heterophase PtPbBi nanosheets (NSs) with a thickness of 2.5 ± 0.3 nm. The oxidative etching effect caused by the coexistence of O2 and Br‒ ions plays a crucial role in the formation of the IMC and unique two-dimensional structure with irregular shapes and curled edges. This study shows that fabricating an A/IMC heterophase structure with a multimetallic composition can effectively enhance the catalytic performances of noble metal-based electrocatalysts.
The development of high-performance, reproducible carbon (C)-based supercapacitors remains a significant challenge because of limited specific capacitance. Herein, we present a novel strategy for fabricating LaCoO x and cobalt (Co)-doped nanoporous C (LaCoO x/Co@ZNC) through the carbonization of Co/Zn-zeolitic imidazolate framework (ZIF) crystals derived from a PVP-Co/Zn/La precursor. The unique ZIF structure effectively disrupted the graphitic C framework, preserved the Co active sites, and enhanced the electrical conductivity. The synergistic interaction between pyridinic nitrogen and Co ions further promoted redox reactions. In addition, the formation of a hierarchical pore structure through zinc sublimation facilitated electrolyte diffusion. The resulting LaCoO x/Co@ZNC exhibited exceptional electrochemical performance, delivering a remarkable specific capacitance of 2,789 F/g at 1 A/g and outstanding cycling stability with 92% capacitance retention after 3,750 cycles. Our findings provide the basis for a promising approach to advancing C-based energy storage technologies.
Cu-based catalysts have been extensively used in methanol steam reforming (MSR) reactions because of their low cost and high efficiency. ZnO is often used in commercial Cu-based catalysts as both a structural and an electronic promoter to stabilize metal Cu nanoparticles and modify metal–support interfaces. Still, the further addition of chemical promoters is essential to further enhance the MSR reaction performance of the Cu/ZnO catalyst. In this work, CeO2-doped Cu/ZnO catalysts were prepared using the coprecipitation method, and the effects of CeO2 on Cu-based catalysts were systematically investigated. Doping with appropriate CeO2 amounts could stabilize small Cu nanoparticles through a strong interaction between CeO2 and Cu, leading to the formation of more Cu+–ZnO x interfacial sites. However, higher CeO2 contents resulted in the formation of larger Cu nanoparticles and an excess of Cu+–CeO x interfacial sites. Consequently, the Cu/5CeO2/ZnO catalyst with maximal Cu–ZnO interfaces exhibited the highest H2 production rate of
Combusting refuse for energy production is promising for their treatment and disposal. However, because of geographical constraints, there has not been a stable model for the energy utilization of refuse in low-oxygen plateau areas. This paper took Lhasa as an example to conduct gasification and incineration experiments on local representative combustible refuse, and relevant energy conversion laws were investigated. Results showed that under gasification and incineration modes, the energy conversion rate of any component of refuse can reach 75% and 85% in low-oxygen plateau areas at temperatures of 450 and 650 °C, respectively, which were 5%–10% lower than those in plain areas. The regional distribution of energy conversion of refuse in Lhasa showed that the energy conversion rate under the gasification mode was 3%–5% lower than that of the incineration mode at 450 and 650 °C. In terms of temperature, the energy conversion rates of refuse were 5%–10% lower at 450 °C than those at 650 °C, but an energy conversion rate of more than 85% can still be achieved. Thus, gasification, incineration, or gasification-assisted secondary incineration at temperatures of at least 450 °C is suitable for energy recovery of refuse in low-oxygen plateau areas.
Cu-based materials are commonly used in electrocatalytic nitrate reduction reactions (NO3RR). NO3RR is a “two birds, one stone” approach, simultaneously removing NO3 − pollutants and producing valuable ammonia (NH3). However, the strong coordination between the NO3 − intermediate and the catalytic active sites seriously hinders the conversion efficiency. Here, we determined that, through encapsulation strategies, the carbon layer could weaken the NO3 − intermediate binding to active sites, resulting in higher NH3 yields. We experimentally fabricated electrocatalysts, i.e., Cu nanoparticles encapsulating (or loaded on) N-doped carbon nanofibers (NCNFs) called Cu@NCNFs (Cu-NCNFs), using electrostatic spinning. As a result, Cu@NCNFs can achieve NH3 yields of 17.08 mg/(h·mgcat) at a voltage of − 0.84 V and a Faraday efficiency of 98.15%. Meanwhile, the electrochemical properties of the Cu nanoparticles on the surface of carbon fibers (Cu-NCNFs) are lower than those of the Cu@NCNFs. The in situ Raman spectra of Cu@NCNFs and Cu-NCNFs under various reduction potentials during the NO3RR process show that catalyst encapsulation within carbon layers can effectively reduce the adsorption of N species by the catalyst, thus improving the catalytic performance in the nitrate-to-ammonia catalytic conversion process.
The strategic manipulation of the interaction between a central metal atom and its coordinating environment in single-atom catalysts (SACs) is crucial for catalyzing the CO2 reduction reaction (CO2RR). However, it remains a major challenge. While density-functional theory calculations serve as a powerful tool for catalyst screening, their time-consuming nature poses limitations. This paper presents a machine learning (ML) model based on easily accessible intrinsic descriptors to enable rapid, cost-effective, and high-throughput screening of efficient SACs in complex systems. Our ML model comprehensively captures the influences of interactions between 3 and 5d metal centers and 8 C, N-based coordination environments on CO2RR activity and selectivity. We reveal the electronic origin of the different activity trends observed in early and late transition metals during coordination with N atoms. The extreme gradient boosting regression model shows optimal performance in predicting binding energy and limiting potential for both HCOOH and CO production. We confirm that the product of the electronegativity and the valence electron number of metals, the radius of metals, and the average electronegativity of neighboring coordination atoms are the critical intrinsic factors determining CO2RR activity. Our developed ML models successfully predict several high-performance SACs beyond the existing database, demonstrating their potential applicability to other systems. This work provides insights into the low-cost and rational design of high-performance SACs.
Flexible strain sensors have received tremendous attention because of their potential applications as wearable sensing devices. However, the integration of key functions into a single sensor, such as high stretchability, low hysteresis, self-adhesion, and excellent antifreezing performance, remains an unmet challenge. In this respect, zwitterionic hydrogels have emerged as ideal material candidates for breaking through the above dilemma. The mechanical properties of most reported zwitterionic hydrogels, however, are relatively poor, significantly restricting their use under load-bearing conditions. Traditional improvement approaches often involve complex preparation processes, making large-scale production challenging. Additionally, zwitterionic hydrogels prepared with chemical crosslinkers are typically fragile and prone to irreversible deformation under large strains, resulting in the slow recovery of structure and function. To fundamentally enhance the mechanical properties of pure zwitterionic hydrogels, the most effective approach is the regulation of the chemical structure of zwitterionic monomers through a targeted design strategy. This study employed a novel zwitterionic monomer carboxybetaine urethane acrylate (CBUTA), which contained one urethane group and one carboxybetaine group on its side chain. Through the direct polymerization of ultrahigh concentration monomer solutions without adding any chemical crosslinker, we successfully developed pure zwitterionic supramolecular hydrogels with significantly enhanced mechanical properties, self-adhesive behavior, and antifreezing performance. Most importantly, the resultant zwitterionic hydrogels exhibited high tensile strength and toughness and displayed ultralow hysteresis under strain conditions up to 1100%. This outstanding performance was attributed to the unique liquid–liquid phase separation phenomenon induced by the ultrahigh concentration of CBUTA monomers in an aqueous solution, as well as the enhanced polymer chain entanglement and the strong hydrogen bonds between urethane groups on the side chains. The potential application of hydrogels in strain sensors and high-performance triboelectric nanogenerators was further explored. Overall, this work provides a promising strategy for developing pure zwitterionic hydrogels for flexible strain sensors and self-powered electronic devices.