Search

The potential of PtS2 with single S-vacancy supported single-atom catalysts as electrocatalysts for CO2 reduction was explored. DFT calculations show that five TM-PtS2 (TM = Sc, V, Fe, Co and Cu) show high catalytic performance.

Iridovirus can cause a mass of death in grouper, leading to huge economic loss in recent years. At present, practical vaccine is still the best way to control the outbreak of this virus. Many researches had indicated that the major capsid protein (MCP) of grouper iridovirus of Taiwan (TGIV) is an effective antigen to induce a specific immune response in grouper. However, these traditional vaccines that based on large proteins or whole organisms are faced with challenges because of the unnecessary antigenic load. Thus, in this study, we screened the dominant linear epitope within the MCP of TGIV and then, a new peptide vaccine (P2) was developed via prokaryotic expression system. Furthermore, SWCNTs was used as a vaccine carrier to enhance the immunoprotective effect. To evaluate the immunoprotective effect of this vaccine, a total of 245 fish were vaccinated with P2 (5, 10, 20 mg L−1) and SWCNTs-P2 (5, 10, 20 mg L−1) via immersion before being challenged with live TGIV at 28 days post immunization (d.p.i.). Results showed that the serum antibody titer, enzymatic activity, expression level of some immune-related genes (CC chemokine, IgM and TNF-α) and survival rate were significantly increased (SWCNTs-P2, 20 mg L−1, 100%) compared to the control group (0%). These results indicated that this peptide vaccine could effectively induce specific immune response in vaccinated groupers. Functionalized SWCNTs could serve as a carrier of the peptide vaccine to enhance the immunoprotective effect via immersion. To sum up, epitope screening might be a potential way to develop an effective vaccine nowadays, and SWCNTs might provide a practical method that can be used in large-scale vaccination, especially for juvenile fish, to fight against diseases in aquaculture industry.

The formation of bimetallic surface alloy catalysts is one of the most promising methods to improve the NO reduction activity of three-way catalysts. Here, the reduction of NO by CO on (100) and (1...

Ever since the concept of superatoms was brought forward in the 1990s, various specific types of clusters have been proposed to mimic atomic properties and enrich the "three-dimensional periodic table". In this work, a Zintl cluster, namely, Ge9Be, has been certified eligible to join the superatom family, owing to its surprising similarity to chalcogen elements. Having 38 valence electrons, Ge9Be has an intrinsic desire to gain two additional electrons to achieve electronic shell closure, in which its quasi-chalcogen identity roots. Like oxygen-group elements, Ge9Be has the potential to form stable ionic compounds with lithium, beryllium, calcium, and superalkaline-earth atom FLi3. On the other hand, the combination of Ge9Be and the multiple valence superatom Al7- results in covalent compounds resembling carbon oxides. Close parallels have also been found between (Ge9Be)2-based compounds and common peroxides, further evidencing the superatom characteristics of Ge9Be. This finding puts forward an almost perfect superatom counterpart of group VIA elements and opens the door to characteristics-oriented design and synthesis of stable superatom motifs by utilizing solid Zintl clusters.

Developing highly efficient and durable eco-friendly heterogeneous catalysts for the Friedel–Crafts acylation (FCA) reaction has been a long-term and significant target, yet remains a great challenge. Herein, a series of Fe–Ni alloy nanoparticles (NPs) encapsulated inside N-doped carbon spheres (FexNi1−x@NC) was rationally fabricated by pyrolyzing the Fe–Ni bimetallic metal–organic frameworks (BMOFs-FexNi1−x) to this end. Various characterization results demonstrated that FeNi alloy NPs (25 nm) covered by a thin carbon shell (5 nm) were uniformly distributed throughout the entire carbon-based composite. A number of oxidized metal species (Fe3+, Ni2+) are present on the surface of the inner bimetallic core, which should be the main source of catalytically active centers of the carbon-wrapped metal NP catalysts. The composition-optimized Fe0.8Ni0.2@NC with relatively higher positive surface charges exhibited the highest catalytic activity and excellent stability for the acylation of aromatic compounds with acyl chlorides. The density functional theory calculations revealed that the catalytic activity of the FexNi1−x@NC catalysts could arise from the electron transfer, i.e., from the outermost layer of the carbon shell to the inner positively charged Fe-based metal NPs, which can lead to a positive charge distribution (by acting as weak Lewis acid sites) on the external surface of the carbon-encapsulated metal NP catalysts. In this case, the external carbon shell can function as ‘chainmail’ to transfer the Lewis acidity (positive charge), and also to protect the inner metal core from the destructive reaction environment, thus resulting in the formation of highly efficient and durable FCA catalysts.

The restructured singly dispersed bimetallic sites M1An supported on the metallic oxide surface have drawn much attention due to their different catalytic performances for the reaction mechanisms o...

The potential of the superalkali cation Li3+ for capturing N2 and its behavior in gaseous nitrogen have been theoretically studied at the MP2/6-311+G(d) level. The evolution of structures and stability of the Li3+(N2)n (n = 1-7) complexes shows that the N2 molecules tend to bind to different vertices of the Li3+ core, and that Li3+ might have the capacity to capture up to twelve nitrogen molecules in the first coordination shell. Based on natural population and molecular orbital analyses, Li3+ keeps its superatom identity in the lowest-lying Li3+(N2)n (n = 1-4) complexes. The change in the Gibbs free energies of possible fragmentation channels also indicates the thermodynamic stability of Li3+ in the (N2)n clusters when n ≤ 4. Different from the case of Li3+(H2O)n, where the electrostatic interaction is dominant, the electrostatic and polarization components are found to make nearly equal contributions to Li3+(N2)n complex formation. In addition, it can be concluded that the superalkali cation Li3+ surpasses heavy alkali metal cations in capturing N2 molecules, since it has a larger binding energy with N2 than Na+ and K+ ions.

The reaction mechanism of bimetallic Pd-Zn-catalyzed cycloaddition of alkynyl aryl ethers with internal alkynes has been studied theoretically. Besides cycloaddition reaction, the dimerization of alkynyl aryl ethers was also considered. Both C6H5OC[triple bond, length as m-dash]CSiiPr3 and C6H5OC[triple bond, length as m-dash]CSiMe3 were chosen as the substrates. The reactions involve C-H activation of the substrate, acetic acid rotation, H transformation, MeC[triple bond, length as m-dash]CMe or substrate insertion into the Pd-phenyl bond and reductive elimination steps. It is found that cycloaddition is favored for C6H5OC[triple bond, length as m-dash]CSiiPr3, while dimerization is preferred for C6H5OC[triple bond, length as m-dash]CSiMe3, because the steric repulsion between two bulky SiiPr3 groups is relatively large and the steric repulsion between two small SiMe3 groups is relatively small. In addition, besides C6H5OC[triple bond, length as m-dash]CSiiPr3, four other substrates C6H5CH2C[triple bond, length as m-dash]CSiiPr3, C6H5C(O)C[triple bond, length as m-dash]CSiiPr3, C6H5SC[triple bond, length as m-dash]CSiiPr3 and C6H5N(H)C[triple bond, length as m-dash]CSiiPr3 have been calculated as the substrates for cycloaddition reaction with MeC[triple bond, length as m-dash]CMe. Among the five substrates, C6H5OC[triple bond, length as m-dash]CSiiPr3 has the lowest energy barrier (29.9 kcal mol-1), consistent with the experimental observation that C6H5OC[triple bond, length as m-dash]CSiiPr3 is the appropriate substrate for successful cycloaddition.

Graphene and many 2D carbon allotropes are good support materials for single-atom catalysts (SACs) and have been successfully applied to many catalytic reactions. Herein, based on the egg tray graphene (ETG), a carbon allotrope constructed in our previous report, we designed ETG and three N-doped ETG supported Pd SACs, Pd@ETG-N x (x= 0–3), for dehydrogenation of formic acid (HCOOH) by density functional theory. Our calculations show that ETG is easier for N doping than graphene, and Pd single atom can be stably adsorbed on the ETG with different N doping concentrations. Major pathways of formic acid dehydrogenation and dehydration were identified. We found that HCOOH dehydrogenation proceeds along the COOH-mediated pathway on each catalyst. With the increased N content in the substrate, the activity and H2 selectivity of Pd SACs are greatly improved. Especially, among these four SACs, Pd@ETG-N3 shows the best catalytic performance, which is even better than Pd(111). Furthermore, electronic analysis was made to reveal the metal-support interactions and the origin of the activity trend of Pd@ETG-N x . Our study reveals the unique potential of carbon allotropes in catalyst design, and provides theoretical insights for rational design of efficient catalysts by adjusting the support and the coordination environment.

We investigate the clinical and genetic characteristics of hemorrhagic cerebrovascular disease in order to provide a new theoretical basis for the prevention and treatment of hereditary cerebrovascular disease.Three hereditary cerebral hemorrhage cases were analyzed retrospectively. The patients' families were surveyed, the clinical characteristics summarized, and gene polymorphisms investigated.Among the three cases, two patients had familial cerebral cavernous hemangiomas, and genetic testing revealed a heterozygous mutation in the CCM1 gene, with a deletion of base (T) in exon 15 (c.1542delT). The last patient had hereditary cerebral hemorrhage with amyloidosis, Finnish type, and the proband, his mother, and his daughter were found to have a heterozygous G duplicate mutation at position 100 in exon 1 of the GSN gene (c.100dupG).Future screening for genetic mutations associated with a high-risk of hereditary cerebral hemorrhage can help identify individuals at risk for this condition and thereby reduce the occurrence and progression of the disease. Such screening will further enhance the precision in preventing and treating cerebrovascular diseases.

The major hindrances of implementing graphene in two-dimensional (2D) electronics are both mechanical (the tendency to crumble and form ripples) and electrical (the lack of a band gap). Moreover, the inevitable structural defects in graphene have a profound influence on its physical and chemical properties. Here, we propose a family of 2D egg-tray graphenes constructed by arranging pentagon and heptagon defects in the graphene lattice based on a careful analysis of the topological distribution of minima, maxima, and saddle points. First-principles calculations show that the egg-tray graphenes are dynamically stable, and their energies, which depend on the concentration of pentagons and heptagons, are the lowest among carbon allotropes. These 2D carbon allotropes exhibit a large variation in their electronic properties, ranging from semimetallic to semiconducting, including some allotropes that have Dirac cones in their band structures. Furthermore, some egg-tray graphenes are predicted to have negative Poisson’s ratios. The adsorption of Li atoms on the egg-tray graphenes is considerably stronger than the adsorption on perfect graphene, therefore they may absorb Li more effectively than graphene, which is important for improving the performance of rechargeable Li batteries.

The reaction mechanism of palladium(0)-catalyzed reaction of aryl iodides, norbornene, and di-tert-butyldiaziridinone has been studied theoretically. Two reaction mechanisms were calculated. The re...

The nitric oxide (NO) reduction by H2 on the pure Ni(110) and single-atom Ir-doped Ni(110) (Ir/Ni(110)) surfaces are investigated by density functional theory calculations coupled with microkinetic...

Noble-metal-free catalysts are highly desirable for hydrogen generation from formic acid dehydrogenation. Herein, using first-principles density functional theory calculations, we design a series of nickel-anchored nitrogenated holey two-dimensional carbon structures (Nix@C2N, x = 1–3) as formic acid dehydrogenation catalysts. For all Nix@C2N surfaces, the formic acid dehydrogenation preferably proceeds via the formate pathway. The effective barrier continuously decreases for formic acid dehydrogenation while increases for hydrogen formation from Ni1@C2N to Ni3@C2N. The side reaction producing carbon monoxide and water via the carboxyl or formyl pathway cannot occur on Ni1@C2N or Ni2@C2N and is not preferred on Ni3@C2N, and thus, the Nix@C2N catalysts possess excellent selectivity of hydrogen. Notably, the unsaturated nitrogen atom of substrate also participates in the reaction and exhibits synergetic effect with the nickel component in Ni1@C2N and Ni2@C2N. The Gibbs free energetic span analysis predicts that the order of reactivity is Ni2@C2N (0.79 eV) > Ni1@C2N (0.87 eV) > Ni3@C2N (1.23 eV), and the turnover frequency of Nix@C2N is evaluated. The results are compared with the experimental and theoretical reports of some palladium-based catalysts. The present work suggests that the Nix@C2N may be promising noble-metal-free catalysts for formic acid dehydrogenation with high performance and low cost.

We employed density functional theory plus the on-site Coulomb repulsion (DFT + U) method to investigate the mechanism of NO reduction with CO on the Co3O4(110)-B and CoO(110) surfaces. The surface...

The potential of the superalkali cation Li3+ for capturing N2 and its behavior in gaseous nitrogen have been theoretically studied at the MP2/6-311+G(d) level. The evolution of structures and stability of the Li3+(N2)n (n = 1-7) complexes shows that the N2 molecules tend to bind to different vertices of the Li3+ core, and that Li3+ might have the capacity to capture up to twelve nitrogen molecules in the first coordination shell. Based on natural population and molecular orbital analyses, Li3+ keeps its superatom identity in the lowest-lying Li3+(N2)n (n = 1-4) complexes. The change in the Gibbs free energies of possible fragmentation channels also indicates the thermodynamic stability of Li3+ in the (N2)n clusters when n ≤ 4. Different from the case of Li3+(H2O)n, where the electrostatic interaction is dominant, the electrostatic and polarization components are found to make nearly equal contributions to Li3+(N2)n complex formation. In addition, it can be concluded that the superalkali cation Li3+ surpasses heavy alkali metal cations in capturing N2 molecules, since it has a larger binding energy with N2 than Na+ and K+ ions.

Spinocerebellar ataxias (SCAs) are a clinically and genetically heterogeneous group accompanied by obvious pontocerebellar limitations. This condition is complex both genetically and phenotypically, making it difficult to describe all the variants simultaneously. Herein, we report a proband from a Chinese mainland family who was admitted to our hospital with paroxysmal limbs jitter and head-shaking. She had experienced broad-based gait, dysarthria, dysmetria, and tremor for about 20 years. Similar clinical symptoms were observed in the daughter, sister and deceased father of this proband. Magnetic resonance imaging showed varying degrees of cerebellar atrophy. The results of whole-exome sequencing (WES) indicated that the three affected members carried the c.590GA mutation in the CCDC88C gene. Based on the diagnosis of SCA40, this proband was treated with aggressive management. Unfortunately, the proband died of suffocation due to laryngeal oedema. Paroxysmal limbs jitter may be a rare phenotype of SCA40 and may occur as a result of involuntary motion which should be differentiated from chorea and epilepsy. In patients with SCA40, pontocerebellar atrophy occurs to varying degrees. Even in the same family, the multiple patients diagnosed did not all exhibit pontocerebellar atrophy. Furthermore, WES is indispensable for the identification of some atypical phenotypes of SCA40.

Supported atomic metal sites have discrete molecular orbitals. Precise control over the energies of these sites is key to achieving novel reaction pathways with superior selectivity. Here, we achieve selective oxygen (O2) activation by utilising a framework of cerium (Ce) cations to reduce the energy of 3d orbitals of isolated copper (Cu) sites. Operando X-ray absorption spectroscopy, electron paramagnetic resonance and density-functional theory simulations are used to demonstrate that a [Cu(I)O2]3− site selectively adsorbs molecular O2, forming a rarely reported electrophilic η2-O2 species at 298 K. Assisted by neighbouring Ce(III) cations, η2-O2 is finally reduced to two O2−, that create two Cu–O–Ce oxo-bridges at 453 K. The isolated Cu(I)/(II) sites are ten times more active in CO oxidation than CuO clusters, showing a turnover frequency of 0.028 ± 0.003 s−1 at 373 K and 0.01 bar PCO. The unique electronic structure of [Cu(I)O2]3− site suggests its potential in selective oxidation., Nature Communications, 11 (1), ISSN:2041-1723

The complexes formed between MgX2 (X = F, H) molecules and alkyl radicals Y [Y = CH3, CH2CH3, CH(CH3)2, and C(CH3)3] have been characterized by using quantum chemical methods. The binding distance in all cases is less than the sum of vdW radii of Mg and C, indicating the formation of a non-covalent interaction, namely single-electron magnesium bond. Energy decomposition analysis reveals that electrostatic and polarization contributions are the major components responsible for the stability of the studied complexes. According to interaction energy, atoms in molecules, and independent gradient model analyses, methyl substitution on electron donor Y imposes a positive effect on its complexation with MgX2. When compared with other nonbonded interactions, the single-electron magnesium bond is found to have strength comparable to those of the single-electron beryllium bond and π-magnesium bond.

Iridovirus of Taiwan (TGIV) has been threatening the grouper farming since 1997, effective prophylaxis method is urgently needed. Subunit vaccine was proved to be useful to against the virus. Bath is the simplest method of vaccination and easy to be administrated without any stress to fish. In this research, we constructed a prokaryotic expression vector of TGIV's major capsid protein (MCP) to acquire the vaccine. Single-walled carbon nanotubes (SWCNTs) were used as the carrier to enhance the protective effect of bath vaccination for juvenile pearl gentian grouper (bath with concentrations of 5, 10, 20 mg/L for 6 h). Virus challenge was done after 28 days. Survival rates were calculated after 14 days. The level of antibody, activities of related enzymes in serums and expression of immune-related genes in kidneys and spleens were test. The results showed that vaccine with SWCNTs as carrier induced a higher level of antibody than that without. In addition, the activities of related enzymes (acid phosphatase, alkaline phosphatase, superoxide dismutase) and the expression of immune-related genes (Mx1, IgM, TNFαF, Lysozyme, CC chemokine 1, IL1-β, IL-8) had a significantly increase. What's more, higher survival rates (42.10%, 77.77%, 89.47%) were provided by vaccine with SWCNTs than vaccine without SWCNTs (29.41%, 38.09%, 43.75%). This study suggests that the protective effect of vaccine that against TGIV with the method of bath vaccination could be enhanced by SWCNTs and SWCNTs could be a potential carrier for other subunit vaccines.

The geometric structures, energetic and electronic properties of global minima of the AlBe n ( n = 1–12) clusters have been systemically studied by using the hybrid density functional theory [B3LYP] and coupled cluster [CCSD(T)] methods. It is found that the impurity Al atom is externally bound to the host Be n framework and its maximum coordination number is six. Besides, the geometries of AlBe n bear close resemblance to either local or global minimum structures of Be n +1 . The AlBe 3 and AlBe 8 clusters exhibit high relative stability among the AlBe n clusters, which is reflected by the evolutions of average atomic binding energy, dissociation energy, second difference in energy, adsorption energy of Al, and HOMO-LUMO gap with cluster size. In comparison to the pure Be n +1 clusters, AlBe n exhibit larger binding energy values, whereas they are more polarizable.

We reported the complete catalytic cycle of dry reforming of methane (DRM) on Ni2Fe overlayer of Ni(1 1 1) surface by periodic density functional theory (DFT) calculations. The pathways for dehydrogenation of CH4 and CO2 activation were located. Our results demonstrate that compared with pure Ni(1 1 1) surface, the introduction Fe into Ni increases the energy barrier of CH dissociation to carbon and hydrogen atoms, thereby suppressing coke deposition on the surface, while it promotes the H-induced CO2 activation pathway to form OH radical, and thus not only the surface oxygen but also OH are responsible for the oxidation of CHx (x = 0,1) on the Ni2Fe overlayer. The most favorable pathway of CH/C oxidation is found to be CH∗ + OH∗ → CHOH∗ → CHO∗ + H∗ → CO∗ + 2H∗, with the rate-limiting energy barrier of 1.12 eV. Furthermore, since Fe is oxidized partially to FeO leading to a partial dealloying under DRM conditions, we also studied the surface-carbon removal and the activity for the reforming of methane on the FeO ribbon supported Ni(1 1 1) (FeO/Ni) interface by DFT+U method. The surface C reacts with lattice oxygen of FeO to produce CO via a Mars−van Krevelen (MvK) mechanism, with a very lower energy barrier of 0.16 eV. The present results show that the introduction of Fe into Ni has a positive effect on the activity toward DRM and has an improved coke resistance.

Compared to noble metals, semiconductor surface enhanced Raman spectrum (SERS) substrates are much cheaper, but their poor sensitivity and stability limits their applications. Here, we report a remarkable enhancement of Raman signals observed from hybrid WO2/C ultrathin nanowire beams. An outstanding enhancement factor (EF) of 1.3 × 106 is achieved, and the lowest detection limit is up to 10−8 M. More importantly, the new SERS active substrate shows ultrahigh chemical, thermal, and light stabilities. An electromagnetic enhancement model and an interfacial charge transfer model coexist in the new SERS substrate.

As a promising hydrotreating catalyst, it was previously reported that Ru⋯OSn (Ru electronically interacts with Sn oxides) on RuSn/SiO2 was the active site for fatty acid hydrogenation, but here in this work we found that Ru3Sn7 nanoclusters on RuSn/SiO2 were responsible for the selective hydrogenation of diverse fatty acids and coconut oil to fatty alcohols. The XPS results indicated no interaction between Snδ+ and Ru0, suggesting that SnOx may exist as isolated species. In contrast, the binding energy shifts of Ru0 and Sn0 in the XPS spectra demonstrated a strong interaction, as a result of the formation of Ru3Sn7 alloy nanoclusters. It was demonstrated that the highest yield of fatty alcohol was obtained with a Sn/Ru ratio of 7/3 (hydrogenation rate: 2.45 g g−1 h−1), and the careful selection of the Sn/Ru ratio and reduction temperatures greatly suppressed the formation of Sn and SnO2 phases. The ratio of the stearyl alcohol formation rate to its consumption rate was 40.8 with Ru3Sn7/SiO2 under the selected conditions. In catalysts with a Sn/Ru ratio higher than 7/3, the presence of additional SnO2 catalyzes the formation of undesired esters at a rate of 0.31 g g−1 h−1. Excess SnO2 would be reduced to Sn at temperatures higher than 600 °C, while Sn can catalyze ester by-product formation at a rate of 0.88 g g−1 h−1. The DFT calculations showed that CH3COOH adsorbs on the Ru3Sn7 (111) surface via Sn–O interactions at the two top sites of adjacent surface Sn atoms, and such adsorption was mainly due to the electrostatic interactions between the molecule and the positively charged surface Sn atoms. The charge density difference (CDD) plots of co-adsorbed CH3CO* and OH* intermediates indicated the bonding relationships between Sn–O and Ru–α-C, suggesting that the surface Sn atoms also took part in the catalytic reaction as an important surface sorption site as well as a Ru3Sn7 structure component, while Ru atoms bonded with α-C and hydrogenated the adsorbed intermediate species with the adsorbed H* to the final alcohol. A further indication that Ru3Sn7 was the active species in the bimetallic Ru–Sn catalyst was given by the much lower energy barrier for hydrogenation of acetic acid in Ru3Sn7 (111) (81.0 kJ mol−1) compared to Ru (0001) (123.5 kJ mol−1).

We have performed a systematic study on the effect of microporosity on the energy stability and electronic properties of graphene-like materials, including 2D C, B and B–C allotropes. We used a modified crystal structure-search method to yield planar structures by systematically varying microporosity. Our results show that the energy stability of allotropes is strongly correlated with the microporosity and that the trends for C and B allotropes are qualitatively different. The formation energies of the most stable C allotropes with the same microporosity increase quickly with the microporosity, which shows a parabolic relationship. In contrast, B allotropes show a much weaker and linear dependence on microporosity. Our calculations also reveal that basic electronic properties such as metallicity and band gaps also depend strongly on the porosity. The allotropes with low microporosity and low formation energies tend to be metallic, and the semiconducting allotropes appear more often with high microporosity. In contrast to the general trend, our study identified a C allotrope with low microporosity that is quite stable and has a large band gap of 0.58 eV.

Fluoromonomers are difficult to polymerize through a coordination mechanism owing to the strong chelation between fluorine and catalysts and the electron-deficient double-bond. We report herein the unprecedented polymerization of para-fluorostyrene (pFS) with excellent activity (1.12×107 g molLn-1 h-1 ), distinguished syndioselectivity (rrrr >99 %) and high conversion (98.4 %) using rare-earth-metal catalysts bearing a pyridyl methylene fluorenyl ligand. DFT calculations reveal polar fluorine loses overwhelming coordination priority to the active central metal ion due to the sterically bulky and electron-donating CGC-ligand, thus its power of poisoning the active species is dramatically weakened. Based on this, copolymerization of pFS and styrene (St) has been successfully achieved with high activity and controllable pFS insertion. Conversely, the unlinked half-sandwich rare-earth-metal system shows relatively lower activity, because both the transition-states and intermediates incorporate a μ1 -F chelated pFS.

Formic acid (HCOOH) is a promising hydrogen carrier. Developing efficient and low-cost catalysts is significant for the application of HCOOH in clean and renewable energy. In this work, a series of single-atom catalysts composed of twelve transition metal single atoms (Mn, Fe, Ru, Co, Rh, Ir, Ni, Pd, Pt, Cu, Ag and Au) supported on a novel carbon-nitrogen material (C3N) were designed and the catalytic performance for HCOOH dehydrogenation was demonstrated using density functional theory. By evaluating the binding strength of TM atoms, the adsorption stability of HCOOH and the hydrogen evolution performance of H species, Ni@C3N, Pd@C3N and Pt@C3N were finally screened out as candidates, on which the HCOO-dehydrogenation pathway is the most preferred. Judging from energetic span, Pd@C3N (0.60 eV) owns the best catalytic activity, while Ni@C3N (1.02 eV) and Pt@C3N (1.12 eV) are also appreciable alternatives compared with Pd( 111) (1.23 eV). Through the analysis of catalytic mechanism and electronic structure, the factors influencing reaction activity were revealed. This work enlightens the advantage of C3N-based materials and provides a novel approach for rationally designing high-performance catalysts for hydrogen production from HCOOH.