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1.
To achieve the energy‐effective ammonia (NH3) production via the ambient‐condition electrochemical N2 reduction reaction (NRR), it is vital to ingeniously design an efficient electrocatalyst assembling the features of abundant surface deficiency, good dispersibility, high conductivity, and large surface specific area (SSA) via a simple way. Inspired by the fact that the MXene contains thermodynamically metastable marginal transition metal atoms, the oxygen‐vacancy‐rich TiO2 nanoparticles (NPs) in situ grown on the Ti3C2Tx nanosheets (TiO2/Ti3C2Tx) are prepared via a one‐step ethanol‐thermal treatment of the Ti3C2Tx MXene. The oxygen vacancies act as the main active sites for the NH3 synthesis. The highly conductive interior untreated Ti3C2Tx nanosheets could not only facilitate the electron transport but also avoid the self‐aggregation of the TiO2 NPs. Meanwhile, the TiO2 NPs generation could enhance the SSA of the Ti3C2Tx in return. Accordingly, the as‐prepared electrocatalyst exhibits an NH3 yield of 32.17 µg h?1 mg?1cat. at ?0.55 V versus reversible hydrogen electrode (RHE) and a remarkable Faradaic efficiency of 16.07% at ?0.45 V versus RHE in 0.1 m HCl, placing it as one of the most promising NRR electrocatalysts. Moreover, the density functional theory calculations confirm the lowest NRR energy barrier (0.40 eV) of TiO2 (101)/Ti3C2Tx compared with Ti3C2Tx or TiO2 (101) alone.  相似文献   

2.
Printing is regarded as a revolutionary and feasible technique to guide the fabrication of versatile functional systems with designed architectures. 2D MXenes are nowadays attractive in printed energy storage devices. However, owing to the van der Waals interaction between the MXene layers, the restacking issues within the printed electrodes can significantly impede the ion/electrolyte transport and hence handicap the electrochemical performances. Herein, a melamine formaldehyde templating method is demonstrated to develop crumpled nitrogen‐doped MXene (MXene‐N) nanosheets. The nitrogen doping boosts the electrochemical performances of MXene via enhanced conductivity and redox activity. Accordingly, two types of MXene‐N inks are prepared throughout the optimization of the ink viscosity to fit the 2D screen printing and 3D extrusion printing, respectively. As a result, the screen printed MXene‐N microsupercapacitor delivers an areal capacitance of 70.1 mF cm?2 and outstanding mechanical robustness. Furthermore, the 3D‐printed MXene‐N based supercapacitor manifests an areal capacitance of 8.2 F cm?2 for a three‐layered electrode and readily stores a high areal energy density of 0.42 mWh cm?2. The approach to harnessing such versatile MXene‐N inks offers distinctive insights into the printed energy storage systems with high areal energy density and large scalability.  相似文献   

3.
The fabrication of fully printable, flexible micro‐supercapacitors (MSCs) with high energy and power density remains a significant technological hurdle. To overcome this grand challenge, the 2D material MXene has garnered significant attention for its application, among others, as a printable electrode material for high performing electrochemical energy storage devices. Herein, a facile and in situ process is proposed to homogeneously anchor hydrous ruthenium oxide (RuO2) nanoparticles on Ti3C2Tx MXene nanosheets. The resulting RuO2@MXene nanosheets can associate with silver nanowires (AgNWs) to serve as a printable electrode with micrometer‐scale resolution for high performing, fully printed MSCs. In this printed nanocomposite electrode, the RuO2 nanoparticles contribute high pseudocapacitance while preventing the MXene nanosheets from restacking, ensuring an effective ion highway for electrolyte ions. The AgNWs coordinate with the RuO2@MXene to guarantee the rheological property of the electrode ink, and provide a highly conductive network architecture for rapid charge transport. As a result, MSCs printed from the nanocomposite inks demonstrate volumetric capacitances of 864.2 F cm?3 at 1 mV s?1, long‐term cycling performance (90% retention after 10 000 cycles), good rate capability (304.0 F cm?3 at 2000 mV s?1), outstanding flexibility, remarkable energy (13.5 mWh cm?3) and power density (48.5 W cm?3).  相似文献   

4.
To enable an efficient and cost‐effective electrocatalytic N2 reduction reaction (NRR) the development of an electrocatalyst with a high NH3 yield and good selectivity is required. In this work, Ti3C2Tx MXene‐derived quantum dots (Ti3C2Tx QDs) with abundant active sites enable the development of efficient NRR electrocatalysts. Given surface functional groups play a key role on the electrocatalytic performance, density functional theory calculations are first conducted, clarifying that hydroxyl groups on Ti3C2Tx offer excellent NRR activity. Accordingly, hydroxyl‐rich Ti3C2Tx QDs (Ti3C2OH QDs) are synthesized as NRR catalysts by alkalization and intercalation. This material offers an NH3 yield and Faradaic efficiency of 62.94 µg h?1 mg?1cat. and 13.30% at ?0.50 V, respectively, remarkably higher than reported MXene catalysts. This work demonstrates that MXene catalysts can be mediated through the optimization of both QDs sizes and functional groups for efficient ammonia production at room temperature.  相似文献   

5.
Crumpled nitrogen‐doped MXene nanosheets with strong physical and chemical coadsorption of polysulfides are synthesized by a novel one‐step approach and then utilized as a new sulfur host for lithium–sulfur batteries. The nitrogen‐doping strategy enables introduction of heteroatoms into MXene nanosheets and simultaneously induces a well‐defined porous structure, high surface area, and large pore volume. The as‐prepared nitrogen‐doped MXene nanosheets have a strong capability of physical and chemical dual‐adsorption for polysulfides and achieve a high areal sulfur loading of 5.1 mg cm–2. Lithium–sulfur batteries, based on crumpled nitrogen‐doped MXene nanosheets/sulfur composites, demonstrate outstanding electrochemical performances, including a high reversible capacity (1144 mA h g–1 at 0.2C rate) and an extended cycling stability (610 mA h g–1 at 2C after 1000 cycles).  相似文献   

6.
As the lightest member of transition metal dichalcogenides, 2D titanium disulfide (2D TiS2) nanosheets are attractive for energy storage and conversion. However, reliable and controllable synthesis of single‐ to few‐layered TiS2 nanosheets is challenging due to the strong tendency of stacking and oxidation of ultrathin TiS2 nanosheets. This study reports for the first time the successful conversion of Ti3C2Tx MXene to sandwich‐like ultrathin TiS2 nanosheets confined by N, S co‐doped porous carbon (TiS2@NSC) via an in situ polydopamine‐assisted sulfuration process. When used as a sulfur host in lithium–sulfur batteries, TiS2@NSC shows both high trapping capability for lithium polysulfides (LiPSs), and remarkable electrocatalytic activity for LiPSs reduction and lithium sulfide oxidation. A freestanding sulfur cathode integrating TiS2@NSC with cotton‐derived carbon fibers delivers a high areal capacity of 5.9 mAh cm?2 after 100 cycles at 0.1 C with a low electrolyte/sulfur ratio and a high sulfur loading of 7.7 mg cm?2, placing TiS2@NSC one of the best LiPSs adsorbents and sulfur conversion catalysts reported to date. The developed nanospace‐confined strategy will shed light on the rational design and structural engineering of metal sulfides based nanoarchitectures for diverse applications.  相似文献   

7.
The 96‐h LC50 (median lethal concentration, LC50) tests were conducted using four different sizes of yellow catfish Pelteobagrus fulvidraco to provide primary information on the sensitivity of this species to elevated ammonia and/or nitrite, and to determine if the sensitivity is mediated by size under the same conditions. The results showed that 96‐h LC50 of fish weighing 0.034 ± 0.002, 0.296 ± 0.049, 3.52 ± 0.95 and 32.96 ± 5.75 g to total ammonia nitrogen‐N was 24.96, 35.85, 47.44 and 68.79 mg L?1, respectively; un‐ionized ammonia nitrogen‐N was 0.34, 0.49, 0.65 and 0.94 mg L?1 in test conditions of pH 7.42 and 23°C; and that nitrite nitrogen‐N was 69.06, 97.23, 133.61 and 196.05 mg L?1 in test conditions of pH 7.58 and 23°C, respectively. The NOEL (No Observable Effect Level) of fish (body weight from 0.03 to 30 g) to ammonia and nitrite was 2.25–6.22 mg L?1 total ammonia nitrogen‐N, 0.03–0.10 mg L?1 un‐ionized ammonia nitrogen‐N in test conditions of pH 7.42 and 23°C, and 6.27–17.68 mg L?1 nitrite nitrogen‐N in test conditions of pH 7.58 and 23°C, respectively. These results indicate that the susceptibility of this fish to total ammonia or nitrite was reduced with increasing size, and that a dose‐dependent relationship might exist between them. The 96‐h LC50 and NOEL of different sizes of fish to total ammonia, un‐ionized ammonia and nitrite would be important to know for water quality standards in yellow catfish aquaculture.  相似文献   

8.
Herein, the authors explicitly reveal the dual‐functions of N dopants in molybdenum disulfide (MoS2) catalyst through a combined experimental and first‐principles approach. The authors achieve an economical, ecofriendly, and most efficient MoS2‐based hydrogen evolution reaction (HER) catalyst of N‐doped MoS2 nanosheets, exhibiting an onset overpotential of 35 mV, an overpotential of 121 mV at 100 mA cm?2 and a Tafel slope of 41 mV dec?1. The dual‐functions of N dopants are (1) activating the HER catalytic activity of MoS2 S‐edge and (2) enhancing the conductivity of MoS2 basal plane to promote rapid charge transfer. Comprehensive electrochemical measurements prove that both the amount of active HER sites and the conductivity of N‐doped MoS2 increase as a result of doping N. Systematic first‐principles calculations identify the active HER sites in N‐doped MoS2 edges and also illustrate the conducting charges spreading over N‐doped basal plane induced by strong Mo 3d –S 2p –N 2p hybridizations at Fermi level. The experimental and theoretical research on the efficient HER catalysis of N‐doped MoS2 nanosheets possesses great potential for future sustainable hydrogen production via water electrolysis and will stimulate further development on nonmetal‐doped MoS2 systems to bring about novel high‐performance HER catalysts.  相似文献   

9.
A copper‐oxide‐based catalyst enriched with paramelaconite (Cu4O3) is presented and investigated as an electrocatalyst for facilitating electroreduction of CO2 to ethylene and other hydrocarbons. Cu4O3 is a member of the copper‐oxide family and possesses an intriguing mixed‐valance nature, incorporating an equal number of Cu+ and Cu2+ ions in its crystal structure. The material is synthesized using a solvothermal synthesis route and its structure is confirmed via powder X‐ray diffraction, transmission electron microscope based selected area electron diffraction, and X‐ray photoelectron spectroscopy. A flow reactor equipped with a gas diffusion electrode is utilized to test a copper‐based catalyst enriched with the Cu4O3 phase under CO2 reduction conditions. The Cu4O3‐rich catalyst (PrC) shows a Faradaic efficiency for ethylene over 40% at 400 mA cm?2. At ?0.64 versus reversible hydrogen electrode, the highest C2+/C1 product ratio of 4.8 is achieved, with C2+ Faradaic efficiency over 61%. Additionally, the catalyst exhibits a stable performance for 24 h at a constant current density of 200 mA cm?2.  相似文献   

10.
Although solid polymer electrolytes have some intrinsic advantages in synthesis and film processing compared with inorganic solid electrolytes, low ionic conductivities and mechanical moduli hamper their practical applications in lithium‐based batteries. Here, an efficient strategy is developed to produce a unique solid polymer electrolyte containing MXene‐based mesoporous silica nanosheets with a sandwich structure, which are fabricated via controllable hydrolysis of tetraethyl orthosilicate around the surface of MXene‐Ti3C2 under the direction of cationic surfactants. Such unique nanosheets not only exhibit individual, thin, and insulated features, but also possess abundant functional groups in mesopores and on the surface, which are favorable for the formation of Lewis acid–base interactions with anions in polymer electrolytes such as poly(propylene oxide) elastomer, enabling the fast Li+ transportation at the mesoporous nanosheets/polymer interfaces. As a consequence, a solid polymer electrolyte with high ionic conductivity of 4.6 × 10?4 S cm?1, high Young's modulus of 10.5 MPa, and long‐term electrochemical stability is achieved.  相似文献   

11.
The detrimental shuttle effect in lithium–sulfur batteries mainly results from the mobility of soluble polysulfide intermediates and their sluggish conversion kinetics. Herein, presented is a multifunctional catalyst with the merits of strong polysulfides adsorption ability, superior polysulfides conversion activity, high specific surface area, and electron conductivity by in situ crafting of the TiO2‐MXene (Ti3C2Tx) heterostructures. The uniformly distributed TiO2 on MXene sheets act as capturing centers to immobilize polysulfides, the hetero‐interface ensures rapid diffusion of anchored polysulfides from TiO2 to MXene, and the oxygen‐terminated MXene surface is endowed with high catalytic activity toward polysulfide conversion. The improved lithium–sulfur batteries deliver 800 mAh g?1 at 2 C and an ultralow capacity decay of 0.028% per cycle over 1000 cycles at 2 C. Even with a high sulfur loading of 5.1 mg cm?2, the capacity retention of 93% after 200 cycles is still maintained. This work sheds new insights into the design of high‐performance catalysts with manipulated chemical components and tailored surface chemistry to regulate polysulfides in Li–S batteries.  相似文献   

12.
A step‐by‐step strategy is reported for improving capacitance of supercapacitor electrodes by synthesizing nitrogen‐doped 2D Ti2CTx induced by polymeric carbon nitride (p‐C3N4), which simultaneously acts as a nitrogen source and intercalant. The NH2CN (cyanamide) can form p‐C3N4 on the surface of Ti2CTx nanosheets by a condensation reaction at 500–700 °C. The p‐C3N4 and Ti2CTx complexes are then heat‐treated to obtain nitrogen‐doped Ti2CTx nanosheets. The triazine‐based p‐C3N4 decomposes above 700 °C; thus, the nitrogen species can be surely doped into the internal carbon layer and/or defect site of Ti2CTx nanosheets at 900 °C. The extended interlayer distance and c‐lattice parameters (c‐LPs of 28.66 Å) of Ti2CTx prove that the p‐C3N4 grown between layers delaminate the nanosheets of Ti2CTx during the doping process. Moreover, 15.48% nitrogen doping in Ti2CTx improves the electrochemical performance and energy storage ability. Due to the synergetic effect of delaminated structures and heteroatom compositions, N‐doped Ti2CTx shows excellent characteristics as an electrochemical capacitor electrode, such as perfectly rectangular cyclic voltammetry results (CVs, R2 = 0.9999), high capacitance (327 F g?1 at 1 A g?1, increased by ≈140% over pristine‐Ti2CTx), and stable long cyclic performance (96.2% capacitance retention after 5000 cycles) at high current density (5 A g?1).  相似文献   

13.
Effects of ammonia stress on food ingestion, growth, digestion and antioxidant capacity were investigated in juvenile yellow catfish Pelteobagrus fulvidraco (Richardson) with initial body weights of 20.24 ± 0.18 g. The fish were reared in triplicate in 15 experimental tanks at a rate of 30 fish per tank for 56 days. Water was maintained at a dissolved oxygen (DO) level of over 6.2 mg L?1, pH 7.2–7.6, and temperature of 29.0 ± 1.5°C under a natural 12L: 12D photoperiod. Survival, food ingestion (FI), specific growth rate (SGR), food conversion efficiency (FCE), apparent digestibility coefficient (ADC), total antioxidant capacity (T‐AOC), levels of glutathione (GSH) and malonaldehyde (MDA), and activities of superoxide dismutase (SOD), catalase (CAT) and glutathione peroxidase (GSH‐PX) of the juveniles were determined in total ammonia nitrogen (NH3‐N+NH4‐N) levels of 0 (control group), 3.36, 6.72, 13.44 and 26.88 mg L?1. The results show that the survival, FI, SGR, FCE, and ADC decreased significantly with an increase in total ammonia nitrogen (p < .05), and a significantly negative correlation between SGR and total ammonia nitrogen levels (p < .05). T‐AOC, SOD, CAT, GSH‐PX and GSH in the blood, liver and gills were found to decline significantly with an increase in the total ammonia nitrogen level (p < .05), while the MDA in the blood, liver and gills was elevated significantly with the increase in total ammonia nitrogen (p < .05). The results indicate a threshold in the induction of the T‐AOC and activities of antioxidant enzymes in yellow catfish tissues with a total ammonia nitrogen increase. In the present study the total ammonia nitrogen threshold thus changed from 6.72 mg L?1 in the juvenile yellow catfish.  相似文献   

14.
Electrochemical CO2 reduction (CO2RR) is a promising technology to produce value‐added fuels and weaken the greenhouse effect. Plenty of efforts are devoted to exploring high‐efficiency electrocatalysts to tackle the issues that show poor intrinsic activity, low selectivity for target products, and short‐lived durability. Herein, density functional theory calculations are firstly utilized to demonstrate guidelines for design principles of electrocatalyst, maximum exposure of catalytic active sites for MoS2 edges, and electron transfer from N‐doped carbon (NC) to MoS2 edges. Based on the guidelines, a hierarchical hollow electrocatalyst comprised of edge‐exposed 2H MoS2 hybridized with NC for CO2RR is constructed. In situ atomic‐scale observation for catalyst growth is performed by using a specialized Si/SiNx nanochip at a continuous temperature‐rise period, which reveals the growth mechanism. Abundant exposed edges of MoS2 provide a large quantity of active centers, which leads to a low onset potential of ≈40 mV and a remarkable CO production rate of 34.31 mA cm?2 with 92.68% of Faradaic efficiency at an overpotential of 590 mV. The long‐term stability shows negligible degradation for more than 24 h. This work provides fascinating insights into the construction of catalysts for efficient CO2RR.  相似文献   

15.
The development of efficient hydrogen evolution reaction electrocatalysts is critical to the realization of clean hydrogen fuel production, while the sluggish kinetics of the Volmer‐step substantially restricts the catalyst performances in alkali electrolyzers, even for noble metal catalysts such as Pt. Here, a Pt‐decorated Ni3N nanosheet electrocatalyst is developed to achieve a top performance of hydrogen evolution in alkaline conditions. Possessing a high metallic conductivity and an atomic‐thin semiconducting hydroxide surface, the Ni3N nanosheets serve as not only an efficient electron pathway without the hindrance of Schottky barriers, but also provide abundant active sites for water dissociation and generation of hydrogen intermediates, which are further adsorbed on the Pt surface to recombine to H2. The Pt‐decorated Ni3N nanosheet catalyst exhibits a hydrogen evolution current density of 200 mA cm?2 at an overpotential of 160 mV versus reversible hydrogen electrode, a Tafel slope of ≈36.5 mV dec?1, and excellent stability of 82.5% current retention after 24 h of operation. Moreover, a hybrid cell consisting of a Pt‐decorated Ni3N nanosheet cathode and a Li‐metal anode is assembled to achieve simultaneous hydrogen evolution and electricity generation, exhibiting >60 h long‐term hydrogen evolution reaction stability and an output voltage ranging from 1.3 to 2.2 V.  相似文献   

16.
2D materials are of particular interest in light‐to‐heat conversion, yet challenges remain in developing a facile method to suppress their light reflection. Herein, inspired by the black scales of Bitis rhinoceros, a generalized approach via sequential thermal actuations to construct biomimetic 2D‐material nanocoatings, including Ti3C2Tx MXene, reduced graphene oxide (rGO), and molybdenum disulfide (MoS2) is designed. The hierarchical MXene nanocoatings result in broadband light absorption (up to 93.2%), theoretically validated by optical modeling and simulations, and realize improved light‐to‐heat performance (equilibrium temperature of 65.4 °C under one‐sun illumination). With efficient light‐to‐heat conversion, the bioinspired MXene nanocoatings are next incorporated into solar steam‐generation devices and stretchable solar/electric dual‐heaters. The MXene steam‐generation devices require much lower solar‐thermal material loading (0.32 mg cm?2) and still guarantee high steam‐generation performance (1.33 kg m?2 h?1) compared with other state‐of‐the‐art devices. Additionally, the mechanically deformed MXene structures enable the fabrication of stretchable and wearable heaters dual‐powered by sunlight and electricity, which are reversibly stretched and heated above 100 °C. This simple fabrication process with effective utilization of active materials promises its practical application value for multiple solar–thermal technologies.  相似文献   

17.
Although the effects of atmospheric nitrogen deposition on species composition are relatively well known, the roles of the different forms of nitrogen, in particular gaseous ammonia (NH3), have not been tested in the field. Since 2002, we have manipulated the form of N deposition to an ombrotrophic bog, Whim, on deep peat in southern Scotland, with low ambient N (wet + dry = 8 kg N ha?1 yr?1) and S (4 kg S ha?1 yr?1) deposition. A gradient of ammonia (NH3, dry N), from 70 kg N ha?1 yr?1 down to background, 3–4 kg N ha?1 yr?1 was generated by free air release. Wet ammonium (NH4+, wet N) was provided to replicate plots in a fine rainwater spray (NH4Cl at +8, +24, +56 kg N ha?1 yr?1). Automated treatments are coupled to meteorological conditions, in a globally unique, field experiment. Ammonia concentrations were converted to NH3‐N deposition (kg N ha?1) using a site/vegetation specific parameterization. Within 3 years, exposure to relatively modest deposition of NH3, 20–56 kg NH3‐N ha?1 yr?1 led to dramatic reductions in species cover, with almost total loss of Calluna vulgaris, Sphagnum capillifolium and Cladonia portentosa. These effects appear to result from direct foliar uptake and interaction with abiotic and biotic stresses, rather than via effects on the soil. Additional wet N by contrast, significantly increased Calluna cover after 5 years at the 56 kg N dose, but reduced cover of Sphagnum and Cladonia. Cover reductions caused by wet N were significantly different from and much smaller than those caused by equivalent dry N doses. The effects of gaseous NH3 described here, highlight the potential for ammonia to destroy acid heathland and peat bog ecosystems. Separating the effects of gaseous ammonia and wet ammonium deposition, for a peat bog, has significant implications for regulatory bodies and conservation agencies.  相似文献   

18.
Supercapacitors attract great interest because of the increasing and urgent demand for environment‐friendly high‐power energy sources. Ti3C2, a member of MXene family, is a promising electrode material for supercapacitors owing to its excellent chemical and physical properties. However, the highest gravimetric capacitance of the MXene‐based electrodes is still relatively low (245 F g?1) and the key challenge to improve this is to exploit more pseudocapacitance by increasing the active site concentration. Here, a method to significantly improve the gravimetric capacitance of Ti3C2Tx MXenes by cation intercalation and surface modification is reported. After K+ intercalation and terminal groups (OH?/F?) removing , the intercalation pseudocapacitance is three times higher than the pristine MXene, and MXene sheets exhibit a significant enhancement (about 211% of the origin) in the gravimetric capacitance (517 F g?1 at a discharge rate of 1 A g?1). Moreover, the as‐prepared electrodes show above 99% retention over 10 000 cycles. This improved electrochemical performance is attributed to the large interlayer voids of Ti3C2 and lowest terminated surface group concentration. This study demonstrates a new strategy applicable to other MXenes (Ti2CTx , Nb2CTx , etc.) in maximizing their potential applications in energy storage.  相似文献   

19.
The photocatalytic reduction of nitrogen (N2) with water (H2O) as the reducing agent holds great promise as a sustainable future technology for the synthesis of ammonia (NH3). Herein, the effect of oxygen vacancies and electron‐rich Cuδ+ on the performance of zinc‐aluminium layered double hydroxide (ZnAl‐LDH) nanosheet photocatalysts for N2 reduction to NH3 under UV–vis excitation is systematically explored. Results show that a 0.5%‐ZnAl‐LDH nanosheet photocatalyst (containing 0.5 mol% Cu by metal basis) affords a remarkable NH3 production rate of 110 µmol g?1 h?1 and excellent stability in pure water. The X‐ray absorption spectroscopy, electron paramagnetic resonance, and density functional theory calculations reveal that Cu addition imparts oxygen vacancies and coordinatively unsaturated Cuδ+ (δ < 2) with electron‐rich property in the ZnAl‐LDH nanosheets, both of which readily contribute to efficient separation and transfer of photogenerated electrons and holes and promote N2 adsorption, thereby both activating N2 and facilitating its multielectrons reduction to NH3.  相似文献   

20.
The electrochemical nitrogen reduction reaction (NRR) is a promising alternative to the energy‐intensive Haber–Bosch process for ammonia synthesis. Among the possible electrocatalysts, bismuth‐based materials have shown unique NRR properties due to their electronic structures and poor hydrogen evolution activity. However, identification of the active sites and reaction mechanism is still difficult due to structural and chemical changes under reaction potentials. Herein, in situ Raman spectroscopy, complemented by electron microscopy, is employed to investigate the structural and chemical transformation of the Bi species during the NRR. Nanorod‐like bismuth‐based metal–organic frameworks are reduced in situ and fragment into densely contacted Bi0 nanoparticles under the applied potentials. The fragmented Bi0 nanoparticles exhibit excellent NRR performance in both neutral and acidic electrolytes, with an ammonia yield of 3.25 ± 0 .08 µg cm?2 h?1 at ?0.7 V versus reversible hydrogen electrode and a Faradaic efficiency of 12.11 ± 0.84% at ?0.6 V in 0.10 m Na2SO4. Online differential electrochemical mass spectrometry detects the production of NH3 and N2H2 during NRR, suggesting a possible pathway through two‐step reduction and decomposition. This work highlights the importance of monitoring and optimizing the electronic and geometric structures of the electrocatalysts under NRR conditions.  相似文献   

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