Recent development of catalytic strategies for sustainable ammonia production

Presently,ammonia is an ideal candidate for future clean energy.The Haber-Bosch process has been an essential ammonia production process,and it is one of the most important technological advancements since its invention,sustaining the explosive growth of military munitions industry and fertilizers in the first half of the 20th century.However,the process is facing great challenges:the growing need for ammonia and the demands of environmental protection.High energy consumption and high CO_(2) emissions greatly limit the application of the Haber-Bosch method,and increasing research efforts are devoted to"green"ammonia synthesis.Thermocatalytic,electrocatalytic,and photocatalytic ammonia production under mild conditions and the derived chemical looping and plasma ammonia production methods,have been widely developed.Electrocatalytic and photocatalytic methods,which use low fossil fuels,are naturally being considered as future directions for the development of ammonia production.Although their catalytic efficiency of ammonia generation is not yet sufficient to satisfy the actual demands,considerable progress has been made in terms of regulating structure and morphology of catalyst and improving preparation efficiency.The chemical looping approach of ammonia production differs from the thermocatalytic,electrocatalytic,and photocatalytic methods,and is the method of reusing raw materials.The plasma treatment approach alters the overall ammonia production approach and builds up a new avenue of development in combination with thermal,photocatalytic,and electrocatalytic methods as well.This review discusses several recent effective catalysts for different ammonia production methods and explores mechanisms as well as efficiency of these catalysts for catalytic N2fixation of ammonia.

Plasma-facilitated modification of pumpkin vine-based biochar and its application for efficient elimination of uranyl from aqueous solution

An acrylic modified pumpkin vine-based biochar(p-PVB-PAA) is synthesized by non-thermal plasma-grafting modification of pumpkin vine-based biochar(PVB) for the removal of uranyl from an aqueous solution. Microscopic characterization reveals that compared to PVB the surface of p-PVBPAA has more oxygen-containing functional groups by strong chemical bonding and the specific surface area is increased to 275.3 m^2 g^-1 from 3.8 m^2g^-1. It is found that p-PVB-PAA showed a much higher maximum adsorption capacity for uranyl from aqueous solutions than PVB, which were207.02 mg g^-1 and 67.58 mg g^-1 at pH=5 and 298 K, respectively. Moreover, the adsorption behavior follows a pseudo-second-order kinetics model and the Langmuir adsorption model.Additionally, macroscopic experiments and spectroscopic studies verified that the significantly improved adsorption performance of the p-PVB-PAA is due to surface complexation and electrostatic interactions. Furthermore, the very high removal efficiency and excellent regeneration ability(the percentage of the removal still remained at nearly 90% after five cycles) makes this low-cost, easily obtained, and environmentally friendly material attractive for commercial application.

Synthesis of novel nanomaterials and their application in efficient removal of radionuclides

With the development of nuclear energy, large amounts of radionuclides are inevitably released into the natural environment. It is necessary to eliminate radionuclides from wastewater for the protection of environment. Nanomaterials have been considered as the potential candidates for the effective and selective removal of radionuclides from aqueous solutions under complicated conditions because of their high specific surface area, large amounts of binding sites, abundant functional groups, pore-size controllable and easily surface modification. This review mainly summarized the recent studies for the synthesis, fabrication and surface modification of novel nanomaterials and their applications in the efficient elimination and solidification of radionuclides,and discussed the interaction mechanisms from batch experiments, spectroscopy analysis and theoretical calculations. The sorption capacities with other materials, advantages and disadvantages of different nanomaterials are compared, and at last the perspective of the novel nanomaterials is summarized.

Nanoscale zero-valent iron/magnetite carbon composites for highly efficient immobilization of U(Ⅵ)

Nanoscale zerovalent iron/magnetic carbon(NZVI/MC) composites were successfully synthesized by simply calcining yellow pine and iron precursors. NZVI/MC pyrolyzed at 800°C(NZVI/MC800) had a higher percentage of NZVI and displayed better resistance to aggregation and oxidation of NZVI than samples prepared at other temperatures. The NZVI/MC800 material was applied for the elimination of U(Ⅵ) from aqueous solutions. The results suggested that the NZVI/MC800 displayed excellent adsorption capacity(203.94 mg/g)toward U(Ⅵ). The significant adsorption capacity and fast adsorption kinetics were attributed to the presence of well-dispersed NZVI, which could quickly reduce U(Ⅵ) into U(Ⅳ), trapping the guest U(Ⅳ) in the porous biocarbon matrix. The removal of U(Ⅵ) on the NZVI/MC samples was strongly affected by solution pH. The NZVI/MC samples also displayed outstanding reusability for U(Ⅵ) removal after multiple cycles. These findings indicate that NZVI/MC has great potential for remediation of wastewater containing U(Ⅵ).

Reductive immobilization of Re(VⅡ)by graphene modified nanoscale zero-valent iron particles using a plasma technique

Technetium-99(~99Tc),largely produced by nuclear fission of ~235U or ~239Pu,is a component of radioactive waste.This study focused on a remediation strategy for the reduction of pertechnetate(Tc O_4^-)by studying its chemical analogue rhenium(Re(VⅡ))to avoid the complication of directly working with radioactive elements.Nanoscale zero-valent iron particles supported on graphene(NZVI/r GOs)from GOs-bound Fe ions were prepared by using a H_2/Ar plasma technique and were applied in the reductive immobilization of perrhenate(Re O_4^-).The experimental results demonstrated that NZVI/r GOs could efficiently remove Re from the aqueous solution,with enhanced reactivity,improved kinetics(50 min to reach equilibrium)and excellent removal capacity(85.77 mg/g).The results of X-ray photoelectron spectroscopy analysis showed that the mechanisms of Re immobilization by NZVI/r GOs included adsorption and reduction,which are significant to the prediction and estimation of the effectiveness of reductive Tc O_4^- by NZVI/r GOs in the natural environment.

Erratum on “Reductive immobilization of Re(Ⅶ) by graphene modified nanoscale zero-valent iron particles using a plasma technique” [Sci.China Chem.,2016,59:150–158]

We regret that our article "Reductive immobilization of Re(Ⅶ) by graphene modified nanoscale zero-valent iron particles using a plasma technique"(Sci. China Chem., 2016, 59:150–158)[1] contained errors. The corrections in an erratum do not change or affect the result or conclusion of the paper.