Efficient adsorption of gaseous radioiodine is pivotal for the sustainable development of nuclear energy and the long-termradiation safety of the ecological system.However,state-of-the-art adsorbents(e.g.metal-organic...Efficient adsorption of gaseous radioiodine is pivotal for the sustainable development of nuclear energy and the long-termradiation safety of the ecological system.However,state-of-the-art adsorbents(e.g.metal-organic frameworks and covalent-organic frameworks)currently under exploration suffer severely from limited adsorption capacity,especially under a real-world scenariowith extremely lowradioiodine concentration and elevated temperature.This mostly originates from the relatively weak sorption driving forces mainly determinedby the iodine-adsorbent interaction consistingof noncovalent interactionswith a small fraction of strong chemical bonding.Here,we document the discovery of an open metal-sulfide framework((NH_(4))_(2)(Sn_(3)S_(7)),donated as SCU-SnS)constructed by three different types of active sites as a superior iodine adsorbent.Benefiting from the ability of iodine for pre-enrichment into the framework by charge-balancing NH_(4)^(+)through N-H···I interaction,the efficient reduction of I^(2)affording I^(-)by S^(2-),and extremely high binding affinity between Sn_(4)^(+)and I^(-),SCU-SnS exhibit a record-breaking iodine adsorption capacity(2.12 g/g)under dynamic breakthrough conditions and the highest static capacity(6.12 g/g)among all reported inorganic adsorbents,both at 348 K.Its facile synthesis and low cost endow SCU-SnS with powerful application potential for the nuclear industry.展开更多
Based on the results of melting experiments on the whole rock of chondrite, the differentiation mechanism of the core, the mantle and the crust of the early Earth was discussed in Ref. [1]. In order to investigate the...Based on the results of melting experiments on the whole rock of chondrite, the differentiation mechanism of the core, the mantle and the crust of the early Earth was discussed in Ref. [1]. In order to investigate the geochemical behaviour of metal-sulfide in the melting-process of the original Earth matter and the formation of the core, further melting experiments were carried out on metal-rich phase of Jilin chondrite under high pressure.展开更多
Sharp interfaces in optoelectronic devices are key for proper band alignment. Despite its benefits as buffer layer, ZnS deposited via atomic layer deposition(ALD) renders intermixed interfaces to its substrate, which ...Sharp interfaces in optoelectronic devices are key for proper band alignment. Despite its benefits as buffer layer, ZnS deposited via atomic layer deposition(ALD) renders intermixed interfaces to its substrate, which can be detrimental for device performance. Here, we are attempting to elucidate the chemical species deriving from this metal-oxide to metal-sulfide transition studying ultrathin film ZnS on SiO_2 using high resolution X-ray photoluminescence spectroscopy(XPS).Regarding the S 2p spectra after a deposition of only three cycles of ZnS, we discover the many different chemical species in which S is present. These include intermediate oxides such as SO_4^(2-).These species become more obvious as we tilt the sample in the XPS chamber to shallower angles.Comparing the Si 2p and S 2p high resolution peaks in the depth profile, one can clearly uncover the confinement of SO_4^(2-) to the interface of the underlying substrate. This may indicate that SiO_2/ZnS interfaces contain interfacial sulphates that likely alter the electronic configuration of this interface.展开更多
We have exploited a new and distinctive combination method that "disperses" elemental Pd into CuS nanoplates. Pd was successfully dispersed by means of the concomitant transformation of CuS into an amorphous sulfide...We have exploited a new and distinctive combination method that "disperses" elemental Pd into CuS nanoplates. Pd was successfully dispersed by means of the concomitant transformation of CuS into an amorphous sulfide, which formed an intimate metal-sulfide contact via cation exchange and underwent a subsequent reduction. A series of such Pd-dispersed CuS hetero-nanoplates were synthesized with tailored proportions and compositions. By efficient utilization of noble metal atoms and stable anchored active sites, the optimal catalytic performance for the semihydrogenation of phenylacetylene, a probe reaction, was achieved with high selectivity, activity, and stability. We believe that the synthetic strategy described in our study is a feasible means of developing effective metal-sulfide catalysts for organic reactions.展开更多
基金The authors gratefully acknowledge the financial support from the National Key R&D Program of China(grant nos.2021YFB3200400 and 2018YFB1900203)the National Natural Science Foundation of China(grant nos.21825601,21790374,22176139,21906113,and 22176163)+2 种基金the Young Taishan Scholars Program(grant no.tsqn201909082)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(grant no.KYCX22_3212)This work is dedicated to Prof.Zhifang Chai on the occasion of his 80th birthday.
文摘Efficient adsorption of gaseous radioiodine is pivotal for the sustainable development of nuclear energy and the long-termradiation safety of the ecological system.However,state-of-the-art adsorbents(e.g.metal-organic frameworks and covalent-organic frameworks)currently under exploration suffer severely from limited adsorption capacity,especially under a real-world scenariowith extremely lowradioiodine concentration and elevated temperature.This mostly originates from the relatively weak sorption driving forces mainly determinedby the iodine-adsorbent interaction consistingof noncovalent interactionswith a small fraction of strong chemical bonding.Here,we document the discovery of an open metal-sulfide framework((NH_(4))_(2)(Sn_(3)S_(7)),donated as SCU-SnS)constructed by three different types of active sites as a superior iodine adsorbent.Benefiting from the ability of iodine for pre-enrichment into the framework by charge-balancing NH_(4)^(+)through N-H···I interaction,the efficient reduction of I^(2)affording I^(-)by S^(2-),and extremely high binding affinity between Sn_(4)^(+)and I^(-),SCU-SnS exhibit a record-breaking iodine adsorption capacity(2.12 g/g)under dynamic breakthrough conditions and the highest static capacity(6.12 g/g)among all reported inorganic adsorbents,both at 348 K.Its facile synthesis and low cost endow SCU-SnS with powerful application potential for the nuclear industry.
基金Project supported by the National Natural Science Foundation of China.
文摘Based on the results of melting experiments on the whole rock of chondrite, the differentiation mechanism of the core, the mantle and the crust of the early Earth was discussed in Ref. [1]. In order to investigate the geochemical behaviour of metal-sulfide in the melting-process of the original Earth matter and the formation of the core, further melting experiments were carried out on metal-rich phase of Jilin chondrite under high pressure.
基金support from Center on Nanostructuring for Efficient Energy Conversion(CNEEC)at Stanford University,an Energy Frontier Research Center funded by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences under Award Number DESC0001060 the Austrian Research Fund(FWF)under the contract J3505-N20
文摘Sharp interfaces in optoelectronic devices are key for proper band alignment. Despite its benefits as buffer layer, ZnS deposited via atomic layer deposition(ALD) renders intermixed interfaces to its substrate, which can be detrimental for device performance. Here, we are attempting to elucidate the chemical species deriving from this metal-oxide to metal-sulfide transition studying ultrathin film ZnS on SiO_2 using high resolution X-ray photoluminescence spectroscopy(XPS).Regarding the S 2p spectra after a deposition of only three cycles of ZnS, we discover the many different chemical species in which S is present. These include intermediate oxides such as SO_4^(2-).These species become more obvious as we tilt the sample in the XPS chamber to shallower angles.Comparing the Si 2p and S 2p high resolution peaks in the depth profile, one can clearly uncover the confinement of SO_4^(2-) to the interface of the underlying substrate. This may indicate that SiO_2/ZnS interfaces contain interfacial sulphates that likely alter the electronic configuration of this interface.
基金The presented research was financially supported by the National Natural Science Foundation of China (Nos. 21325101, 21231005, and 21171105).
文摘We have exploited a new and distinctive combination method that "disperses" elemental Pd into CuS nanoplates. Pd was successfully dispersed by means of the concomitant transformation of CuS into an amorphous sulfide, which formed an intimate metal-sulfide contact via cation exchange and underwent a subsequent reduction. A series of such Pd-dispersed CuS hetero-nanoplates were synthesized with tailored proportions and compositions. By efficient utilization of noble metal atoms and stable anchored active sites, the optimal catalytic performance for the semihydrogenation of phenylacetylene, a probe reaction, was achieved with high selectivity, activity, and stability. We believe that the synthetic strategy described in our study is a feasible means of developing effective metal-sulfide catalysts for organic reactions.