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1.
Inorg Chem ; 2024 Aug 22.
Article in English | MEDLINE | ID: mdl-39172735

ABSTRACT

Integrated application of interface engineering and vacancy engineering is a promising and effective strategy for the design and fabrication of high-performance electrocatalysts. Herein, the heterointerface catalyst with rich sulfur vacancies, vs-Ni3S2/Fe2P, was successfully designed and constructed. The strong heterointerface coupling and rich sulfur vacancies in vs-Ni3S2/Fe2P significantly optimize the electronic structure of the catalyst and synergistically improve the inherent catalytic activity. Benefiting from the optimization of the electronic structure, vs-Ni3S2/Fe2P exhibits excellent bifunctional electrocatalytic performance in alkaline electrolytes. The overpotentials for hydrogen and oxygen evolution reactions (HER and OER) are 99 and 169 mV at a current density of 10 mA cm-2, respectively. Particularly, it achieves an ultrahigh OER performance with an overpotential of 251 mV at 300 mA cm-2. Moreover, the catalyst also displays outstanding long-term durability. Density functional theory (DFT) computations reveal that the synergy of interface coupling and sulfur vacancies is crucial to optimizing the electronic structure. This study offers a hopeful pathway for the design and construction of durable and efficient electrocatalysts.

2.
Article in English | MEDLINE | ID: mdl-39073348

ABSTRACT

OBJECTIVE: Chronic low back pain (cLBP) affects nociceptive responses in the cerebellum, which leads to increased pain perception and sensorimotor control dysfunction. This study aimed to investigate altered functional connectivity in the anterior and posterior lobes of the cerebellum during cLBP. DESIGN: Twenty patients with cLBP and 18 healthy participants underwent 3.0 T resting-state functional magnetic resonance imaging. The bilateral lobule V of the anterior cerebellum and Crus I of the posterior cerebellum were selected as the region of interest for identifying the corresponding networks. RESULTS: The left lobule V had a greater intrinsic connectivity with the left insular cortex, left orbitofrontal cortex, and bilateral medial prefrontal cortex in patients with cLBP. In contrast, the right lobule V and bilateral Crus I had a significantly decreased connectivity with the contralateral multimodal cerebral networks, including the default mode network, salience network, and emotional network. CONCLUSION: The cerebellum had mechanistic implications in pain-related changes, which are involved in motor control, cognition, and emotion processing. These findings provide a novel perspective on the role of functional subregions in cLBP, which add to the growing body of evidence that the cerebellum can be a potential target for noninvasive brain stimulation for chronic pain treatment.

3.
Chem Sci ; 15(26): 10046-10055, 2024 Jul 03.
Article in English | MEDLINE | ID: mdl-38966385

ABSTRACT

Materials exhibiting highly efficient, ultralong and multicolor-tunable room-temperature phosphorescence (RTP) are of practical importance for emerging applications. However, these are still very scarce and remain a formidable challenge. Herein, using precise structure design, several novel organic-inorganic metal-halide hybrids with efficient and ultralong RTP have been developed based on an identical organic cation (A). The original organic salt (ACl) exhibits red RTP properties with low phosphorescence efficiency. However, after embedding metals into the organic salt, the changed crystal structure endows the resultant metal-halide hybrids with excellent RTP properties. In particular, A2ZnCl4·H2O exhibits the highest RTP efficiency of up to 56.56% with a long lifetime of up to 159 ms. It is found that multiple inter/intramolecular interactions and the strong heavy-atom effect of the rigid metal-halide hybrids can suppress molecular motion and promote the ISC process, resulting in highly stable and localized triplet excitons followed by highly efficient RTP. More crucially, multicolor-tunable fluorescence and RTP achieved by tuning the metal and halogen endow these materials with wide application prospects in the fields of multilevel information encryption and dynamic optical data storage. The findings promote the development of phosphorescent metal-halide hybrids for potential high-tech applications.

4.
Article in English | MEDLINE | ID: mdl-38969254

ABSTRACT

OBJECTIVE: To investigate the neural mechanism underlying functional reorganization and motor coordination strategies in patients with chronic low back pain (cLBP). DESIGN: A case-control study based on data collected during routine clinical practice. SETTING: This study was conducted at a university hospital. PARTICIPANTS: Fifteen patients with cLBP and 15 healthy controls. INTERVENTIONS: Not applicable. MAIN OUTCOME MEASURES: Whole brain blood oxygen level-dependent signals were measured using functional magnetic resonance imaging and amplitude of low-frequency fluctuation (ALFF) method to identify pain-induced changes in regional spontaneous brain activity. A novel approach based on the surface electromyogram (EMG) system and fine-wire electrodes was used to record EMG signals in the deep multifidus, superficial multifidus, and erector spinae. RESULTS: In cLBP, compared with healthy groups, ALFF was higher in the medial prefrontal, primary somatosensory, primary motor, and inferior temporal cortices, whereas it was lower in the cerebellum and anterior cingulate and posterior cingulate cortices. Furthermore, the decrease in the average EMG activity of the 3 lumbar muscles in the cLBP group was positively correlated with the ALFF values of the primary somatosensory cortex, motor cortex, precuneus, and middle temporal cortex but significantly negatively correlated with the ALFF values of the medial prefrontal and inferior temporal cortices. Interestingly, the correlation between the functional activity in the cerebellum and the EMG activity varied in the lumbar muscles. CONCLUSIONS: These findings suggest a functional association between changes in spontaneous brain activity and altered voluntary neuromuscular activation patterns of the lumbar paraspinal muscles, providing new insights into the mechanisms underlying pain chronicity as well as important implications for developing novel therapeutic targets of cLBP.

5.
Small ; : e2312122, 2024 May 06.
Article in English | MEDLINE | ID: mdl-38709229

ABSTRACT

Management of functional groups in hole transporting materials (HTMs) is a feasible strategy to improve perovskite solar cells (PSCs) efficiency. Therefore, starting from the carbazole-diphenylamine-based JY7 molecule, JY8 and JY9 molecules are incorporated into the different electron-withdrawing groups of fluorine and cyano groups on the side chains. The theoretical results reveal that the introduction of electron-withdrawing groups of JY8 and JY9 can improve these highest occupied molecular orbital (HOMO) energy levels, intermolecular stacking arrangements, and stronger interface adsorption on the perovskite. Especially, the results of molecular dynamics (MD) indicate that the fluorinated JY8 molecule can yield a preferred surface orientation, which exhibits stronger interface adsorption on the perovskite. To validate the computational model, the JY7-JY9 are synthesized and assembled into PSC devices. Experimental results confirm that the HTMs of JY8 exhibit outstanding performance, such as high hole mobility, low defect density, and efficient hole extraction. Consequently, the PSC devices based on JY8 achieve a higher PCE than those of JY7 and JY9. This work highlights the management of the electron-withdrawing groups in HTMs to realize the goal of designing HTMs for the improvement of PSC efficiency.

6.
J Colloid Interface Sci ; 670: 132-141, 2024 Sep 15.
Article in English | MEDLINE | ID: mdl-38759268

ABSTRACT

Developing simple and energy-saving pathways to prepare high-efficient and robust non-noble metal based electrocatalysts remains a huge challenge to hydrogen production from seawater electrolysis. Here we demonstrate a facile hydrothermal-calcination-etching approach that simultaneously achieves the required surface N doping and Fe vacancies generation to activate the Ni-O-Fe active motifs in N-vFe-NiFe2O4/NF. The unique localized environments (Ni-N-Fe structures and unsaturated O- and N-coordination) due to dual-defect strategy can effectively regulate the electronic structure of the Ni-O-Fe motif to make the motif more reactive. As a result, the N-vFe-NiFe2O4/NF catalyst exhibits overpotentials of 210, 213 and 222 mV to deliver 100 mA cm-2 in 1.0 M KOH, simulated seawater and alkaline seawater environments, respectively. Theoretical calculations prove that the Ni-O-Fe structure is the active motif and that the presence of special localized environments can optimize the adsorption of key intermediates on the activated active motifs.

7.
Inorg Chem ; 63(22): 10335-10345, 2024 Jun 03.
Article in English | MEDLINE | ID: mdl-38768637

ABSTRACT

Low-dimensional lead-halide hybrids are an emerging class of optical functional material but suffer the problems of toxicity and poor air stability. Among lead-free metal halides, tin(IV)-based metal halides are promising optoelectronic materials due to their robust structure and environmental friendliness. However, their photoluminescence (PL) properties are poor, and the underlying mechanisms are still elusive. Herein, a stable Sn4+-based halide hybrid, (C4H7N2)2SnCl6, was developed, which however exhibits poor PL properties at room temperature (RT) due to the lattice defects and the robust crystal structure. To enhance its PL efficiency, the Te4+ ion with a stereoactive 5s2 lone pair has been introduced into the lattice. As a result, Te4+-doped (C4H7N2)2SnCl6 displays broadband orange emission (∼640 nm) with a PL efficiency of ∼46% at RT. Interestingly, Te4+-doped (C4H7N2)2SnCl6 shows triple emission bands at 80 K, which could be due to the synergistic effect of the organic cations and the self-trapped state induced by Te4+. Additionally, high-performance white light-emitting diodes were prepared using Te4+-doped (C4H7N2)2SnCl6, revealing the potential of this material for lighting applications. This study provides new insight into the PL mechanism of Sn4+-based metal-halide hybrids and thus facilitates the design and development of eco-friendly light-emitting metal halides.

8.
Inorg Chem ; 63(13): 5821-5830, 2024 Apr 01.
Article in English | MEDLINE | ID: mdl-38511502

ABSTRACT

A highly luminescent (C13H28N2)2Cu4I8 single crystal containing isolated γ-[Cu4I8]4- anionic cluster was synthesized without the use of unsaturated cations. To the best of our knowledge, compounds bearing such like anions are not dual-emitting under UV excitation. However, dual emission does occur in (C13H28N2)2Cu4I8. Moreover, the emission bands were found to be temperature-sensitive, allowing tuning of the emission colors from blue (0.19, 0.20) to green (0.33, 0.47) in the Commission International de L' Eclairage (CIE) chromaticity coordinates. Remarkably, the color could be restored on returning to the initial temperature, confirming an efficient and reversible luminescent thermochromic effect in (C13H28N2)2Cu4I8. The origin of this excellent optical performance is discussed, and the difference in the mechanism with the dual-emissive Cu(I) halide complexes is also elucidated. Overall, our work provides a promising way to achieve efficient luminescent thermochromism. The developed (C13H28N2)2Cu4I8 represents one of the viable alternatives for eco-friendly luminescent thermochromic materials.

9.
Inorg Chem ; 63(11): 5158-5166, 2024 Mar 18.
Article in English | MEDLINE | ID: mdl-38456436

ABSTRACT

Low-dimensional hybrid metal halides are an emerging class of materials with highly efficient photoluminescence (PL), but the problems of poor stability remain challenging. Sn(IV)-based metal halides show robust structure but exhibit poor PL properties, and the structure-luminescence relationship is elusive. Herein, two Sn(IV)-based metal halides (compounds 1 and 2) with the same constituent ((C6H16N2)SnCl6) but different crystal structures have been prepared, which however show poor PL properties at room temperature due to the absence of active ns2 electrons. To improve materials' PL properties, Sb3+ with active 5s2 electrons was embedded into the lattice of Sn4+-based hosts. As a result, efficient emissions were achieved for Sb3+-doped compounds 1 and 2 with a maximum PL efficiency of 14.28 and 62%, respectively. Experimental and calculation results reveal that the smaller distorted lattice structure of the host could result in the blueshift of the emission from Sb3+. Thus, a tunable color from red to orange was realized. Benefiting from the broadband efficient emission from Sb3+-doped compound 2, an efficient white light-emitting diode with a high color rendering index of up to 92.3 was fabricated to demonstrate its lighting application potential. This work promotes the understanding of the influence of robust Sn(IV)-based host lattice on the PL properties of Sb3+, advancing the development of environmentally friendly, low-cost, and high-efficiency Sn(IV)-based metal halides.

10.
Small ; 20(33): e2400859, 2024 Aug.
Article in English | MEDLINE | ID: mdl-38516951

ABSTRACT

Active and stable nonnoble electrocatalysts for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are required for water splitting by sustainable electricity. Here, Mn bonded with O and P is incorporated to modulate Co3S4 and Co2P respectively to enhance the catalytic activity and extend the catalyst lifetime. Mn3O4 adjusts the electronic structure of Co3S4 and Co atom fills the oxygen vacancy in Mn3O4. The interfacial interaction endows Co3S4/Mn3O4 to a lower reaction barrier due to ideal binding energies for OER intermediates. Structure stability of active sites and enhanced Co─S bonds by Operando Raman spectroscopy and theoretical calculations reduce the dissolution of Co3S4/Mn3O4, resulting in a lifetime of 500 h at 50 mA cm-2 for OER. The modulation of Co2P by MnP weakens the interaction between Co sites and adsorbed H*, achieving a high activity under a large current for HER. The assembled electrolyzer affords 50 mA cm-2 at 1.58 V and exhibits a lifetime of 350 h at 50 mA cm-2. The calculations disclose the electron interaction for the activity and stability, as well as the enhanced conductivity. The findings develop new avenues toward promoting catalytic activity and stability, making Co─Mn bimetallic nanowires efficient electrocatalysts for nonnoble water electrolyzers.

11.
Small ; 20(26): e2310387, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38312084

ABSTRACT

Rational design of heterostructure catalysts through phase engineering strategy plays a critical role in heightening the electrocatalytic performance of catalysts. Herein, a novel amorphous/crystalline (a/c) heterostructure (a-CoS/Ni3S2) is manufactured by a facile hydrothermal sulfurization method. Strikingly, the interface coupling between amorphous phase (a-CoS) and crystalline phase (Ni3S2) in a-CoS/Ni3S2 is much stronger than that between crystalline phase (c-CoS) and crystalline phase (Ni3S2) in crystalline/crystalline (c/c) heterostructure (c-CoS/Ni3S2) as control sample, which makes the meta-stable amorphous structure more stable. Meanwhile, a-CoS/Ni3S2 has more S vacancies (Sv) than c-CoS/Ni3S2 because of the presence of an amorphous phase. Eventually, for the oxygen evolution reaction (OER), the a-CoS/Ni3S2 exhibits a significantly lower overpotential of 192 mV at 10 mA cm-2 compared to the c-CoS/Ni3S2 (242 mV). An exceptionally low cell voltage of 1.51 V is required to achieve a current density of 50 mA cm-2 for overall water splitting in the assembled cell (a-CoS/Ni3S2 || Pt/C). Theoretical calculations reveal that more charges transfer from a-CoS to Ni3S2 in a-CoS/Ni3S2 than in c-CoS/Ni3S2, which promotes the enhancement of OER activity. This work will bring into play a fabrication strategy of a/c catalysts and the understanding of the catalytic mechanism of a/c heterostructures.

12.
J Colloid Interface Sci ; 656: 137-145, 2024 Feb 15.
Article in English | MEDLINE | ID: mdl-37988781

ABSTRACT

Electrochemical reduction of contaminated nitrate to ammonia (NRA) opens a new window for mass production of ammonia and the alleviation of energy crises and environmental pollution. However, fabricating effective catalysts for the NRA still faces significant challenges. Herein, a highly-efficient NRA catalyst, FeP4/Ni2P, was successfully constructed. The strong electron coupling at heterointerfaces of FeP4/Ni2P promoted the generation of abundant active hydrogen *H, inhibited the competition of the HER, accelerated the hydrogenation of the NRA. Benefiting from these, the catalyst displays good NRA catalytic activity in the neutral electrolyte, with the NH3 FE of 97.83 ± 0.091 %, NH3 selectivity of 98.67 ± 0.50 %, NH3 yield rate of 0.262 ± 0.01 mmol·h-1·cm-2, and NO3- conversion rate of 93.02 ± 0.14 %. The DFT theoretical calculations demonstrated that the FeP4/Ni2P heterointerfaces played a critical role in shearing the H-OH bonds of water, resulting in generating more active hydrogen as a key NRA hydrogenation source, and hindering the *H dimerization to form H2, enhancing the NH3 selectivity. This work has a certain reference value for designing excellent catalysts for the NRA.

13.
Mater Horiz ; 10(12): 5633-5642, 2023 Nov 27.
Article in English | MEDLINE | ID: mdl-37753534

ABSTRACT

It is a promising pathway to use anions to regulate electronic structures, reasonably design and construct highly efficient catalysts for water splitting. Herein, a N-regulated Co cluster catalyst confined in carbon nanotubes, N-Co NCNTs, was constructed successfully. Nitrogen anions played a crucial role in optimizing the electronic structures of Co clusters and enhancing localization of electrons, resulting in polarized cobalt clusters. The N-induced electronic localization and the resulting polarized Co clusters are responsible for the improvement of catalytic activity. N-Co NCNTs exhibited ultra-low overpotentials of 178 mV and 92 mV for the OER and HER to achieve 10 mA cm-2 in an alkaline electrolyte, respectively. Its long-term catalytic durability is mainly attributed to the obstacle to the surface oxidation of Co clusters caused by N-regulation. N-Co NCNTs maintained a stable current density for 160 h at 10 mA cm-2. DFT computations confirmed the decisive role played by nitrogen anions in regulating the electronic structure. This work provides a pathway for understanding and designing highly efficient anion-regulated catalysts.

14.
Chem Sci ; 14(21): 5665-5671, 2023 May 31.
Article in English | MEDLINE | ID: mdl-37265737

ABSTRACT

The direct catalytic α-hydrocarbylation of readily available amino acids with halohydrocarbons is one of the most straightforward methods leading to α,α-disubstituted non-proteinogenic α-amino acid compounds. However, all the reported methodologies depend on N-protected amino acids as starting materials. Herein, we report on three highly efficient aldehyde-catalyzed direct α-hydrocarbylations of N-unprotected amino acid esters with aryl-, allyl-, and benzyl halides. By promoting a simple chiral BINOL-aldehyde catalyst or combining catalysts of a chiral aldehyde and Lewis acid ZnCl2, the asymmetric α-arylation, α-allylation, and α-benzylation of amino acid esters with the corresponding halohydrocarbons proceed smoothly, producing α,α-disubstituted α-amino acids in moderate-to-high yields and good-to-excellent enantioselectivities. The asymmetric α-arylation reaction can be applied in the formal synthesis of the clinical candidate compound (+)-AG-041R. Based on the results given by control experiments, three reaction models are proposed to illustrate the stereoselective-control outcomes.

15.
Chem Sci ; 14(20): 5415-5424, 2023 May 24.
Article in English | MEDLINE | ID: mdl-37234888

ABSTRACT

Designing and synthesizing cuprous halide phosphors unifying efficient low-energy emission and a broad excitation band is still a great challenge. Herein, by rational component design, three novel Cu(i)-based metal halides, DPCu4X6 [DP = (C6H10N2)4(H2PO2)6; X = Cl, Br, I], were synthesized by reacting p-phenylenediamine with cuprous halide (CuX), and they show similar structures, consisting of isolated [Cu4X6]2- units separated by organic layers. Photophysical studies uncover that the highly localized excitons and rigid environment give rise to highly efficient yellow-orange photoluminescence in all compounds with the excitation band spanning from 240 to 450 nm. The bright PL in DPCu4X6 (X = Cl, Br) originates from self-trapped excitons due to the strong electron-phonon coupling. Intriguingly, DPCu4I6 features a dual-band emissive characteristic, attributed to the synergistic effect of halide/metal-to-ligand charge-transfer (X/MLCT) and triplet cluster-centered (3CC) excited states. Benefiting from the broadband excitation, a high-performance white-light emitting diode (WLED) with a high color rendering index of 85.1 was achieved using single-component DPCu4I6 phosphor. This work not only unveils the role of halogens in the photophysical processes of cuprous halides, but also provides new design principles for high-performance single-component WLEDs.

16.
J Colloid Interface Sci ; 643: 563-573, 2023 Aug.
Article in English | MEDLINE | ID: mdl-37031070

ABSTRACT

Lithium-sulfur batteries (LSBs) is a promising secondary battery system with high energy density and environment-friendly characteristics, however, the severe "shuttle effect" and poor conductivity usually lead to short service life and low initial capacity. Carbon Nanotubes (CNTs) with excellent conductivity and large quantity of cavities are promising host materials, whereas, the weak interaction between CNTs and polysulfides usually leads to serious shuttle effect in charge/discharge processes. Herein, thienothiophene-based covalent organic framework is uniformly wrapped on the outer surface of CNTs to form a nanocomposite TT-BOST@CNT. It is observed that the coexistence of the electron-rich S, O and the electron-deficient B atoms enables the effective adsorption of both Li+ and Sx2- in lithium polysulfides (LiPSs). Studies reveal that the B, O and S atoms endow the nanocomposite with good catalysis ability, whereby, conversion of the insoluble long-chain polysulfides to the soluble short-chain polysulfides is accelerated. Consequently, the TT-BOST@CNT/S cathode displays outstanding electrochemical performance, with a high discharge specific capacity of 1545 mAh g-1 at 0.2 C and a small attenuation rate of 0.035% per cycle in 1000 cycles at 1 C.

17.
Inorg Chem ; 62(2): 1054-1061, 2023 Jan 16.
Article in English | MEDLINE | ID: mdl-36606542

ABSTRACT

The zero-dimensional (0D) (H5O2)(C4H14N2S2)2BiCl8: Sb3+ single crystal is obtained by the cooling crystallization method. Surprisingly, this compound shows reversible photoluminescence (PL) upon H5O2+Cl- removal and insertion. To be specific, the release of H5O2+Cl- resulted in red-orange emission with a very low photoluminescence quantum yield (PLQY). While on the reuptake of it, a bright yellow emission with a nearly 10-fold increase of PLQY was observed. Density functional theory (DFT) calculations and temperature-dependent PL experiments reveal that significant [SbCl6]3- octahedron distortion induced by guest (H5O2+Cl-) removal at the ground state, especially at the excited state, is responsible for the disparate PL performance. Encouragingly, we also found that (C4H14N2S2)2BiCl7: Sb3+ exhibits a fast response (<3 s) to dilute hydrochloric acid with naked-eye perceivable PL color changes, rendering it a potential sensing material for hydrochloric acid.

18.
Inorg Chem ; 62(6): 2806-2816, 2023 Feb 13.
Article in English | MEDLINE | ID: mdl-36716166

ABSTRACT

ns2-Metal halide perovskites have attracted wide attention due to their fascinating photophysical properties. However, achieving high photoluminescence (PL) properties is still an enormous challenge, and the relationship between the lattice environment and ns2-electron expression is still elusive. Herein, an organic-inorganic Bi3+-based halide (C5H14N2)2BiCl6·Cl·2H2O (C5H14N22+ = doubly protonated 1-methylpiperazine) with a six-coordinated structure has been successfully prepared, which, however, exhibits inferior PL properties due to the chemically inert expression of Bi3+-6s2 lone-pair electrons. After reasonably embedding Sb3+ with 5s2 electrons into the lattice of (C5H14N2)2BiCl6·Cl·2H2O, the host lattice environment induces the Sb-Cl moiety to change from the original five-coordinated to six-coordinated structure, thereby resulting in a broad-band yellow emission with a PL efficiency up to 50.75%. By utilizing the host lattice of (C5H14N2)2BiCl6·Cl·2H2O, the expression of Sb3+-5s2 lone-pair electrons is improved and thus promotes the radiative recombination from the Sb3+-3P1 state, resulting in the enhanced PL efficiency. This work will provide an in-depth insight into the effect of the local structure on the expression of Sb3+-5s2 lone-pair electrons.

19.
J Colloid Interface Sci ; 633: 189-198, 2023 Mar.
Article in English | MEDLINE | ID: mdl-36446211

ABSTRACT

Understanding the synergistic mechanism of multi-component alloys is crucial and challenging for overall water splitting. Herein, Ru-NiCo0.5-600 °C and Ru-Ni0.75Co with excellent electrocatalytic activity are designed and synthesized. The Ru-NiCo0.5-600 °C alloy exhibits remarkable HER activity with an overpotential of 42, 77 and 93 mV at 10 mA cm-2 in alkaline, acidic and neutral conditions, and the Ru-Ni0.75Co electrocatalyst presents outstanding OER activity with an overpotential of 176 mV at 10 mA cm-2 in 1.0 M KOH. The Ru-NiCo0.5-600 °C ||Ru-Ni0.75Co cell requires only 1.48 and 1.69 V to reach 10 and 100 mA cm-2 towards overall water splitting. A series of experiments reveal that the strong electronic coupling among Ru, Ni and Co regulates the electronic structure and enhances the intrinsic catalytic activity and stability of the as-synthesized Ru-NiCo electrocatalysts. Systematic experimental and theoretical results prove that Ni atoms act as the active sites of dissociating water, while Ru and Co are respectively the active centers of proton and hydroxyl adsorption for HER and OER. Our work provides a new perspective for profoundly understanding the synergistic effect of multi-component alloys towards water splitting.


Subject(s)
Alloys , Electronics , Adsorption , Hydroxyl Radical , Water
20.
ChemSusChem ; 16(7): e202201892, 2023 Apr 06.
Article in English | MEDLINE | ID: mdl-36541588

ABSTRACT

Herein, vanadium-doped cobalt carbonate hydroxide, V-CoCH, was synthesized as efficient catalyst for water splitting. Vanadium species were partially dissolved in the early stages of the oxygen-evolution reaction (OER), inducing self-etching of the catalyst surface, which is helpful for catalyst surface reconstruction and resulted in a higher number of active sites and oxygen vacancies. The synergy between V-doping and oxygen vacancies improved the catalytic activity: V-CoCH showed an exceptional OER catalytic performance with an overpotential of 183 mV at 10 mA cm-2 . The water-splitting cell consisting of V-CoCH only required 1.52 V to reach 10 mA cm-2 . Theoretical calculations revealed that vanadium in V-CoCH played an important role in electron regulation of active sites. The oxygen vacancies had an important effect on improvement of the OER performance through not only the exposure of more active sites but also through modulation of the electronic structure. This work provides an effective strategy for constructing high-performance electrocatalysts.

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