Temperature-programmed Desorption Results Research Articles

Constructing Mo5+ sites in molybdenum oxide by lattice stress for efficient ammonia synthesis

Molybdenum oxide (MoO3) is a promising catalyst for electrocatalytic nitrogen reduction (eNRR). However, Mo sites with saturated coordination are not favorable to stable N2 adsorption. Herein, we employed sodium ions as electron donors to interact with the interlayer atoms of MoO3, causing localized lattice stress on it and weakening the M-O bond, thus inducing the Mo5+ active sites (NaxMoO3). The N2 temperature-programmed desorption (N2-TPD) result of the as-prepared NaxMoO3 exhibits that introducing Mo5+ could significantly improve the N2 adsorption on the catalyst’s surface. The optimized NaxMoO3 has an NH3 yield of 41.3 μg h−1 mg−1 at ambient temperature and an FE of 21.4 %, which is in the relatively advanced position in the contemporaneous studies. Both experiments and density-functional theory (DFT) calculation demonstrated that the Mo5+ sites can effectively reduce the d-orbital energy level of Mo, which significantly enhances the interaction with N2.

Cu@Co with Dilatation Strain for High-Performance Electrocatalytic Reduction of Low-Concentration Nitric Oxide.

Electrocatalytic reduction of nitric oxide (NO) to ammonia (NH3 ) is a clean and sustainable strategy to simultaneously remove NO and synthesize NH3 . However, the conversion of low concentration NO to NH3 is still a huge challenge. In this work, the dilatation strain between Cu and Co interface over Cu@Co catalyst is built up and investigated for electroreduction of low concentration NO (volume ratio of 1%) to NH3 . The catalyst shows a high NH3 yield of 627.20µg h-1 cm-2 and a Faradaic efficiency of 76.54%. Through the combination of spherical aberration-corrected transmission electron microscopy and geometric phase analyses, it shows that Co atoms occupy Cu lattice sites to form dilatation strain in the xy direction within Co region. Further density functional theory calculations and NO temperature-programmed desorption (NO-TPD) results show that the surface dilatation strain on Cu@Co is helpful to enhance the NO adsorption and reduce energy barrier of the rate-determining step (*NO to *NOH), thereby accelerating the catalytic reaction. To simultaneously realize NO exhaust gas removal, NH3 green synthesis, and electricity output, a Zn-NO battery with Cu@Co cathode is assembled with a power density of 3.08mW cm-2 and an NH3 yield of 273.37µg h-1 cm-2 .

Direct Visualization of CO Interaction on Oxygen Poisoned Co(0001).

The poisoning of catalysts has always been a vital issue in catalytic reactions. In this study, direct observation of the interaction of CO and oxygen-poisoned Co(0001) has been achieved with scanning tunneling microscopy (STM), temperature-programmed desorption (TPD), and density functional theory calculation. A two-stage adsorption process of CO on a well-prepared p(2×2)-O layer covered Co(0001) was directly visualized. With increasing annealing time at a certain temperature after the CO dosage, the ordered (2 × 2) pattern formed in the first stage can be recovered, suggesting the weak interaction of CO with the O-covered Co(0001) surface in the latter stage. Compared to the clean Co(0001) surface, on an oxygen-poisoned surface, no further reaction was observed, illustrating the poisoning of the catalyst. Moreover, TPD results are in good agreement with the STM observation; a desorption energy of 0.35 eV is evaluated with a simple but accurate scheme.

Origin of Higher CO Oxidation Activity of Pt/Rutile than That of Pt/Anatase

Herein, we show that the weak interaction of CO with Pt/TiO2 under the CO oxidation condition is the origin of higher CO oxidation activity of Pt/rutile than that of Pt/anatase. The results of CO temperature-programmed desorption (TPD) and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) indicate that the onset temperatures of CO desorption on freshly prepared Pt/rutile and Pt/anatase are the same. However, the CO-TPD curves of Pt/rutile after the reaction test show that the desorption temperature of CO shifts to a lower temperature, while that for Pt/anatase does not change. The in situ pulse reaction using DRIFTS reveals that CO on Pt/rutile reacted with oxygen faster than CO on Pt/anatase. IR spectra with peak deconvolution of adsorbed CO on Pt/rutile exhibit that CO adsorbed on the terrace sites of Pt clusters on rutile (2089 cm–1) reacts readily with O2. These results indicate that the higher low-temperature activity of Pt/rutile is related to its weaker interaction with CO compared with Pt/anatase under the reaction conditions. Our findings deepen the fundamental understanding of metal–support interaction and CO oxidation on Pt/TiO2 catalysts.

Synthesis, characterization, and application of bio-templated Ni–Ce/Al2O3 catalyst for clean H2 production in the steam reforming of methane process

A mesoporous γ-alumina was successfully synthesized through an environmentally-friendly method using Fig leaves as a bio-template for the first time in this research. After confirming the formation of porous Al2O3 structure with different characterization techniques, it was used as a supporting material of Ni–Ce particles to effectively enhance the conversion of steam reforming of methane (SRM) process. For this purpose, we optimized Ni content, Ce content, and SRM temperature using bulk and porous structure of Ni–Ce/Al2O3 catalysts. The results of field emission scanning electron microscopy (FESEM), temperature-programmed desorption (H2-TPD), and N2 adsorption/desorption showed the formation of more dispersed Ni particles with smaller sizes on the mesoporous alumina (MAl), especially when they were promoted with CeO2. Besides the efficient influence of CeO2 on Ni particle dispersion, it was enhanced the Ni–Al interaction, increased the activity of the catalysts, and decreased the coke deposition on the catalysts during the SRM process. As a result, 20Ni-3.0Ce/MAl catalyst depicted the highest H2 yield of 96.02% and CH4 conversion of 90.20%, and the lowest produced CO2 to consumed CH4 of 0.52% at 700 °C SRM reaction. This is while the bulky catalyst with equal Ni and Ce contents had 86.09, 92.30, and 0.56 CH4 conversion, H2 yield, and CO2/CH4 molar ratio, respectively at this temperature. Besides, 20Ni-3.0Ce/MAl depicted the highest stability during 12 h continuous SRM reaction at 700 °C with the lowest reduction amounts of 3.97% and 5.12% for CH4 conversion and H2 yield, respectively.

Stepwise photoassisted decomposition of carbohydrates to H2

Stepwise photoassisted decomposition of carbohydrates to H2

Low-temperature NH3-SCR performance of a novel Chlorella@Mn composite denitrification catalyst

The synthesis process of conventional Mn-based denitrification catalysts is relatively complex and expensive. In this paper, a resource application of chlorella was proposed, and a Chlorella@Mn composite denitrification catalyst was innovatively synthesized by electrostatic interaction. The Chlorella@Mn composite denitrification catalyst prepared under the optimal conditions (0.54 g/L Mn2+ concentration, 20 million chlorellas/mL concentration, 450°C calcination temperature) exhibited a well-developed pore structure and large specific surface area (122 m2/g). Compared with MnOx alone, the Chlorella@Mn composite catalyst achieved superior performance, with ∼100% NH3 selective catalytic reduction (NH3-SCR) denitrification activity at 100-225°C. The results of NH3 temperature-programmed desorption (NH3-TPD) and H2 temperature-programmed reduction (H2-TPR) showed that the catalyst had strong acid sites and good redox properties. Zeta potential testing showed that the electronegativity of the chlorella cell surface could be used to enrich with Mn2+. X-ray photoelectron spectroscopy (XPS) confirmed that Chlorella@Mn had a high content of Mn3+ and surface chemisorbed oxygen. In-situ diffuse reflectance infrared Fourier transform spectroscopy (in-situ DRIFTS) experimental results showed that both Langmuir-Hinshelwood (L-H) and Eley-Rideal (E-R) mechanisms play a role in the denitrification process on the surface of the Chlorella@Mn catalyst, where the main intermediate nitrate species is monodentate nitrite. The presence of SO2 promoted the generation and strengthening of Brønsted acid sites, but also generated more sulfate species on the surface, thereby reducing the denitrification activity of the Chlorella@Mn catalyst. The Chlorella@Mn composite catalyst had the characteristics of short preparation time, simple process and low cost, making it promising for industrial application.

Na Promotion of Pt/m-ZrO2 Catalysts for the Steam Reforming of Formaldehyde

The decomposition selectivity of formaldehyde during steam reforming was explored using unpromoted and sodium promoted Pt/m-ZrO2 catalysts, and the Na content was varied (0.5%Na, 1%Na, 1.8%Na, 2.5%Na, and 5%Na). In situ DRIFTS experiments during temperature programmed reaction in flowing H2O revealed that formaldehyde is adsorbed at reduced defect sites on zirconia, where it is converted to formate species through the addition of labile bridging OH species. Formate species achieve a maximum intensity in the range of 125–175 °C, where only slight changes in intensity are observed. Above this temperature, the formate decomposition reactivity strongly depends on the Na loading, with the optimum loadings being 1.8%Na and 2.5%Na. CO2 temperature programmed desorption results, as well as a greater splitting observed between the formate νasym(OCO) and νsym(OCO) bands in infrared spectroscopy, indicate greater basicity is induced by the presence of Na. This strengthens the interaction between the formate -CO2 functional group and the catalyst surface, weakening the formate C-H bond. A shift in the ν(CH) band of formate to lower wavenumbers was observed by addition of Na, especially at 1.8%Na and higher loadings. This results in enhanced decarboxylation and dehydrogenation of formate, as observed in in situ DRIFTS, temperature-programmed reaction/mass spectrometry experiments of the steam reforming of formaldehyde, and fixed bed reaction tests. For example, 2.5%Na addition of 2.5% increased the CO2 selectivity from 83.5% to 99.5% and the catalysts achieved higher stable conversion at lower temperature than NiO catalysts reported in the open literature. At 5%Na loading, Pt sites were severely blocked, hindering H-transfer.

Experimental study of the catalytic effect of iron on low-rank coal gasification

Acid-washing low-rank coal samples were loaded with different content of iron catalyst and then pyrolyzed. FT-IR, Raman spectra, and temperature-programmed experiments were used to investigate the influence of iron on the coal char. The FT-IR results revealed that iron catalyst rises the number of –OH, –CH3, and –CH2 functional groups. The Raman spectra results showed that partial large polyaromatic ring structures transform into small polyaromatic ring structures after the addition of iron. The results of temperature-programmed desorption indicated that the number of surface active sites is increased due to the addition of iron. For low-rank coal char with 3% Fe, the number of active sites increased with the increase of adsorption temperature until 800 °C and then start to decrease. At 750 °C, the adsorption capacity of CO2 increased with the increase of time and reached saturation state after 45 min. The results of the char-steam isothermal gasification experiment suggested that the iron catalyst enhances the gasification reactivity of low-rank coal. It is verified that iron catalysts can improve the gasification reactivity of low-rank coal by increasing the number of surface active sites.

Contribution of Na/K Doping to the Activity and Mechanism of Low-Temperature COS Hydrolysis over TiO2-Al2O3 Based Catalyst in Blast Furnace Gas

As an organic sulfur pollutant generated in blast furnace gas, carbonyl sulfide (COS) has attracted more attention due to its negative effects on the environment and economy. The TiO2-Al2O3 composite metal oxide (Ti0.5Al) with uniformly dispersed particles was prepared by the co-precipitation method. And on this basis, a series of Na/K-doped catalysts were prepared separately. The activity evaluation results showed that the introduction of Na/K significantly improved the low-temperature COS hydrolysis activity, which exhibited a COS conversion of 98% and H2S yield of 95% at 75 °C with 24,000 h–1. And K showed a better promoting effect than Na. Brunauer–Emmett–Teller (BET) results revealed the increased mesopore proportion of Na/K-modified catalysts. X-ray diffraction (XRD) and scanning electron microscopy (SEM) showed that Na and K formed prismatic and nanorod-like structures, respectively. More weakly basic sites with enhanced intensity and decreased Oads/Olat content contributed to the excellent catalytic activity, as certified by the results of CO2 temperature-programmed desorption (CO2-TPD) and X-ray photoelectron spectroscopy (XPS). It was also proposed that the decrease of weakly basic sites ultimately deactivated catalyst activity. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) showed that the introduction of Na/K enhanced the dissociation of H2O, and the generated abundant hydroxyl groups promoted the adsorption of COS and formed surface transition species, such as HSCO2– and HCO3–.

Strain-assisted in-situ formed oxygen defective WO3 film for photothermal-synergistic reverse water gas shift reaction and single-particle study

Among the reactions about CO2 conversion, the reverse water gas shift (RWGS) reaction is an efficient method to convert CO2 to CO. Herein, by the assistance of strain and introduction of light and reactant, in-situ formed oxygen defective WO3 film was synthesized, as an effective catalyst for reverse water gas shift reaction with an intense photothermal-synergistic effect. Furthermore, the in-situ single-particle Time-Resolved Photoluminescence (TRPL) and Photoluminescence (PL) spectrum were used to explore the details during the reaction, and prolonged charge carrier lifetime and significantly enhanced Photoluminescence intensities were observed in the in-situ single-particle study. Notably, the production rate of CO for WO3 film is almost 10 times that of powder, which means that WO3 film has an intense photothermal-synergistic effect. As proved by the results of CO2 temperature-programmed desorption (TPD) and CO2 adsorption, the oxygen vacancies are beneficial to the capture and activation of CO2, boosting the process of the reverse water gas shift. Meanwhile, lattice strain arising from the thermal expansion during the reaction could assist the in-situ formation of oxygen defects, enhance charge separation and regulate the electrical structure. All of this contribute to the synergy effect in photothermal reaction. Our work may provide a novel strategy for reasonable design of catalyst and illuminate the behavior of carriers in single-particle level.

Efficient degradation of multiple Cl-VOCs by catalytic ozonation over MnOx catalysts with different supports

This paper investigated catalytic ozonation of different Cl-VOCs (chlorobenzene (CB), dichloroethane (DCE), dichloromethane (DCM) and trichloroethylene (TCE)) over series of supported MnOx catalysts.These Cl-VOCs with different molecule structures exhibited obviously difference in catalytic performances and byproducts formation. Interestingly, the correlation between catalytic behaviors and surface properties of catalysts was inconsistent for different Cl-VOCs. In comparison, Mn/HZSM-5(27) presented a better conversion and mineralization rate (MAR) for most of Cl-VOCs due to its abundant surface acidity and excellent pore structures. Catalytic co-ozonation of mixed Cl-VOCs over Mn/HZSM-5(27) showed co-existence of inhibitive and promotive effects. For instance, CB conversion occupied priority compared with DCE and TCE, and MAR was enhanced in the mixture. Thereafter, the temperature programmed desorption results of mixed Cl-VOCs proved competitive adsorption between molecules. Both competitive adsorption and difficulty of Cl-VOCs degradation were the determining factors in catalytic co-ozonation of Cl-VOCs. Besides, catalytic co-ozonation of Cl-VOCs with presence of H2O exhibited negligible impact. These observations provide valuable reference for industrial application with co-presence of multiple Cl-VOCs and water vapor.

Low-temperature Hg0 abatement by ionic liquid based on weak interaction

Low-temperature gaseous elemental mercury (Hg0) abatement is an objective demand in industrial flue gas treatment. In this work, we proposed a new approach for Hg0 capture via weak interaction of ionic liquids. Ionic liquids with varied anions (1-butyl-3-methylimidazolium thioacetate ([Bmim][ThAc]), 1-butyl-3-methylimidazolium diethyldithiocarbamate ([Bmim][DTCR]), and 1-butyl-3-methylimidazolium ethylxanthate ([Bmim][EX])) were designed and synthesized. The interaction energies between ionic liquids and elemental mercury were proved to be positively related to mercury removal efficiency, revealing that the electrostatic interaction derived physical adsorption from anions is the dominant factor affecting mercury removal performance. [Bmim][ThAc] with the largest anionic electrostatic interaction energy showed the best mercury abatement performance, achieving a Hg0 removal efficiency of over 98% and an adsorption capacity of 10.66 mg/g at 50 °C. The influence of temperature and the results of mercury temperature-programmed desorption (Hg-TPD), X-ray photoelectron spectroscopy (XPS) further confirmed that the ionic liquid combines with elemental mercury through physical adsorption. The work provides a new perspective on designing high-efficiency sorbents for mercury removal at low temperature.

Temperature‐Dependent CO2 Electroreduction over Fe‐N‐C and Ni‐N‐C Single‐Atom Catalysts

AbstractReaction temperature is an important parameter to tune the selectivity and activity of electrochemical CO2 reduction reaction (CO2RR) due to different thermodynamics of CO2RR and competitive hydrogen evolution reaction (HER). In this work, temperature‐dependent CO2RR over Fe‐N‐C and Ni‐N‐C single‐atom catalysts are investigated from 303 to 343 K. Increasing the reaction temperature improves and decreases CO Faradaic efficiency over Fe‐N‐C and Ni‐N‐C catalysts at high overpotentials, respectively. CO current density over Fe‐N‐C catalyst increases with temperature, then gets into a plateau at 323 K, finally reaches the maximum value of 185.8 mA cm−2 at 343 K. While CO current density over Ni‐N‐C catalyst achieves the maximum value of 252.5 mA cm−2 at 323 K, and then drops significantly to 202.9 mA cm−2 at 343 K. Temperature programmed desorption results and density functional theory calculations reveal that the difference of temperature‐dependent variation on CO Faradaic efficiency and current density between Fe‐N‐C and Ni‐N‐C catalysts results from the varied adsorption strength of key reaction intermediates during CO2RR.

Temperature-Dependent CO2 Electroreduction over Fe-N-C and Ni-N-C Single-Atom Catalysts.

Reaction temperature is an important parameter to tune the selectivity and activity of electrochemical CO2 reduction reaction (CO2 RR) due to different thermodynamics of CO2 RR and competitive hydrogen evolution reaction (HER). In this work, temperature-dependent CO2 RR over Fe-N-C and Ni-N-C single-atom catalysts are investigated from 303 to 343 K. Increasing the reaction temperature improves and decreases CO Faradaic efficiency over Fe-N-C and Ni-N-C catalysts at high overpotentials, respectively. CO current density over Fe-N-C catalyst increases with temperature, then gets into a plateau at 323 K, finally reaches the maximum value of 185.8 mA cm-2 at 343 K. While CO current density over Ni-N-C catalyst achieves the maximum value of 252.5 mA cm-2 at 323 K, and then drops significantly to 202.9 mA cm-2 at 343 K. Temperature programmed desorption results and density functional theory calculations reveal that the difference of temperature-dependent variation on CO Faradaic efficiency and current density between Fe-N-C and Ni-N-C catalysts results from the varied adsorption strength of key reaction intermediates during CO2 RR.

Effect of synthesis method on the ultimate properties of copper-based catalysts supported on KIT-6 for direct CO2 hydrogenation to methanol

The effect of synthesis method on the ultimate properties of copper-based catalysts supported on KIT-6 was investigated. A series of catalysts with 0.60Cu/0.15ZnO/0.05MnO/1.0KIT-6 mole ratio was synthesized using three methods, i.e. citric acid impregnation (CA), wet impregnation (WI), and deposition-precipitation (DP). Characterization study shows the catalyst synthesized using CA method had relatively high metal-support interactions and preserved the structures of preshaped KIT-6 support the best. The CA catalyst was also characterized with low mesopore plugging, high porosity, along with the formation of small copper crystallites and large copper surface areas. The presence of abundant accessible active sites in CA catalyst is strongly supported by temperature-programmed desorption results. After reaction, X-ray diffraction analysis indicates CA catalyst had greatest resistance to copper crystallite growth. In direct CO2 hydrogenation reaction, the CA catalyst led to remarkably high methanol production rate (3.94 kg/kgcat·h), i.e. 34%–164% higher than the others, including a commercial catalyst.

DFT and Experimental Studies on the Mechanism of Mercury Adsorption on O2-/NO-Codoped Porous Carbon.

The utilization of O2 and NO in flue gas to activate the raw porous carbon with auxiliary plasma contributes to an effective mercury (Hg)-removal strategy. The lack of in-depth knowledge on the Hg adsorption mechanism over the O2-/NO-codoped porous carbon severely limits the development of a more effective Hg removal method and the potential application. Therefore, the generation processes of functional groups on the surface during plasma treatment were investigated and the detailed roles of different groups in Hg adsorption were clarified. The theoretical results suggest that the formation of functional groups is highly exothermic and they preferentially form on a carbon surface, and then affect Hg adsorption. The active groups affect Hg adsorption in a different manner, which depends on their nature. All of these active groups can improve Hg adsorption by enhancing the interaction of Hg with a surface carbon atom. Particularly, the preadsorbed NO2 and O3 groups can react directly with Hg by forming HgO. The experimental results confirm that the active groups cocontribute to the high Hg removal efficiency of O2-/NO-codoped porous carbon. In addition, the mercury temperature-programmed desorption results suggest that there are two forms of mercury present on O2-/NO-codoped porous carbon, including a carbon-bonded Hg atom and HgO.

Hydrocracking of Polyethylene to Jet Fuel Range Hydrocarbons over Bifunctional Catalysts Containing Pt- and Al-Modified MCM-48

A low-density polyethylene was hydrocracked to liquid hydrocarbons in autoclave reactors over catalysts containing Pt- and Al-modified MCM-48. Two kinds of Al-modified MCM-48 were synthesized for the reaction: Al-MCM-48 was synthesized using a sol–gel method by mixing Al(iso-OC3H7)3 with Si(OC2H5)4 and surfactant in a basic aqueous solution before hydrothermal synthesis, and Al/MCM-48 was synthesized using a post-modification method by grafting Al3+ ions on the surface of calcined Al/MCM-48. X-ray diffraction (XRD) patterns indicated that both Al-MCM-48 and Al/MCM-48 had a cubic mesoporous structure. The Brunauer–Emmett–Teller (BET) surface areas of Al-MCM-48 and Al/MCM-48 were larger than 1000 m2/g. 27Al Magic Angle Spinning-NMR (MAS NMR) indicated that Al3+ in Al-MCM-48 was located inside the framework of mesoporous silica, but Al3+ in Al/MCM-48 was located outside the framework of mesoporous silica. The results of ammonia temperature-programmed desorption (NH3-TPD) showed that the acidic strength of various samples was in the order of H-Y > Al/MCM-48 > Al-MCM-48 > MCM-48. After 4 MPa H2 was charged in the autoclave at room temperature, 1 wt % Pt/Al/MCM-48 catalyst showed a high yield of C9−C15 jet fuel range hydrocarbons of 85.9% in the hydrocracking of polyethylene at 573 K for 4 h. Compared with the reaction results of Pt/Al/MCM-48, the yield of light hydrocarbons (C1−C8) increased over Pt/H-Y, and the yield of heavy hydrocarbons (C16−C21) increased over Pt/Al-MCM-48 in the hydrocracking of polyethylene. The yield of C9−C15 jet fuel range hydrocarbons over the used catalyst did not decrease compared to the fresh catalyst in the hydrocracking of polyethylene to jet fuel range hydrocarbons over Pt/Al/MCM-48.

Hydrotalcite-assisted rapid synthesis of HKUST-1 toward efficient benzene capture

Volatile organic compounds (VOCs) have been recognized as one of the major environmental hazards in the air. Metal organic frameworks (MOFs) and their associated materials have offered an excellent strategy for the adsorption removal of VOCs. In this work, we develop a facile and rapid synthesis method of HKUST-1, a typical and ideal Cu-based MOF, for VOC adsorption by using hydrotalcite as the intermediate for efficient crystallization at room temperature. The results show that HKUST-1 can be successfully synthesized within 10 s at room temperature. The as-synthesized HKUST-1 has a Brunauer-Emmett-Teller surface area of 2170.7 m2 g−1 and a total pore volume of 0.977 cm3 g−1, which are among the highest reported values for such material. When tested for its benzene adsorption performance, the material can achieve a saturated adsorption capacity of 7.3 mmol g−1 at 35 °C. Based on the temperature-programmed desorption result, it is shown that the activation energy for the benzene desorption is 68.23 kJ mol−1. The material can demonstrate a relatively constant saturated adsorption capacity after several adsorption/desorption cycles, which indicates good regenerative performance.

Exploring N-Containing Compound Catalyst for H2S Selective Oxidation: Case Study of TaON and Ta3N5

In addition to traditional metal oxides, N-containing compound would become efficient catalyst for H2S selective oxidation. TaON and Ta3N5, taking as examples, with porous structure are able to selectively oxidize H2S into sulfur. TaON exhibits ca. 99% H2S conversion and ca. 89% sulfur selectivity at 250 ℃, while Ta3N5 exhibits near complete H2S conversion (~ 100%) and 86% sulfur selectivity at 250 ℃. TaON of lower N content shows higher sulfur selectivity (~ 90–100%) above 130 ℃, compared with that (~ 86–95%) over Ta3N5. Whereas, Ta3N5 of higher N content demonstrates higher H2S conversion (~ 30–40%) below 160 ℃, compared with that (~ 6–30%) over TaON. Temperature programmed desorption results show that Ta3N5 owns larger amount of acid sites and weaker basic sites than TaON. Over Ta3N5, the reactant molecules could dissociatively adsorb on acid sites more frequently and could be easier to move across the weaker basic sites, thus increasing probability for reaction at low temperature. Manipulating both cations and anions in N-containing compound can alter surface property for optimization of selective H2S oxidation.