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Conductive catalysis by subsurface transition metals.

ABSTRACT: The nature of catalysis has been hotly pursued for over a century, and current research is focused on understanding active centers and their electronic structures. Herein, the concept of conductive catalysis is proposed and verified by theoretical simulations and experimental observations. Metallic systems containing buried catalytically active transitional metals and exposed catalytically inert main group metals are constructed, and the electronic interaction between them via metallic bonding is disclosed. Through the electronic interaction, the catalytic properties of subsurface transitional metals (Pd or Rh) can be transferred to outermost main group metals (Al or Mg) for several important transformations like semi-hydrogenation, Suzuki-coupling and hydroformylation. The catalytic force is conductive, in analogy with the magnetic force and electrostatic force. The traditional definition of active centers is challenged by the concept of conductive catalysis and the electronic nature of catalysis is more easily understood. It might provide new opportunities for shielding traditional active centers against poisoning or leaching and allow for precise regulation of their catalytic properties by the conductive layer.

SUBMITTER: Deng X

PROVIDER: S-EPMC10849361 | biostudies-literature | 2024 Jan

REPOSITORIES: biostudies-literature

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Conductive catalysis by subsurface transition metals.

Deng Xin X Zheng Caiyan C Li Yangsheng Y Zhou Zeyu Z Wang Jiamin J Ran Yihua Y Hu Zhenpeng Z Yang Fan F Li Landong L

National science review 20240111 1

The nature of catalysis has been hotly pursued for over a century, and current research is focused on understanding active centers and their electronic structures. Herein, the concept of conductive catalysis is proposed and verified by theoretical simulations and experimental observations. Metallic systems containing buried catalytically active transitional metals and exposed catalytically inert main group metals are constructed, and the electronic interaction between them <i>via</i> metallic bo ...[more]

PMID: 38328681

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Project description:This study employed 16S rRNA gene amplicon pyrosequencing to examine the hypothesis that chemolithotrophic Fe(II)-oxidizing bacteria (FeOB) would preferentially colonize the Fe(II)-bearing mineral biotite compared to quartz sand when the minerals were incubated in situ within a subsurface redox transition zone (RTZ) at the Hanford 300 Area site in Richland, WA, USA. The work was motivated by the recently documented presence of neutral-pH chemolithotrophic FeOB capable of oxidizing structural Fe(II) in primary silicate and secondary phyllosilicate minerals in 300 Area sediments and groundwater (Benzine et al., 2013). Sterilized portions of sand+biotite or sand alone were incubated in situ for 5 months within a multilevel sampling (MLS) apparatus that spanned a ca. 2-m interval across the RTZ in two separate groundwater wells. Parallel MLS measurements of aqueous geochemical species were performed prior to deployment of the minerals. Contrary to expectations, the 16S rRNA gene libraries showed no significant difference in microbial communities that colonized the sand+biotite vs. sand-only deployments. Both mineral-associated and groundwater communities were dominated by heterotrophic taxa, with organisms from the Pseudomonadaceae accounting for up to 70% of all reads from the colonized minerals. These results are consistent with previous results indicating the capacity for heterotrophic metabolism (including anaerobic metabolism below the RTZ) as well as the predominance of heterotrophic taxa within 300 Area sediments and groundwater. Although heterotrophic organisms clearly dominated the colonized minerals, several putative lithotrophic (NH4 (+), H2, Fe(II), and HS(-) oxidizing) taxa were detected in significant abundance above and within the RTZ. Such organisms may play a role in the coupling of anaerobic microbial metabolism to oxidative pathways with attendant impacts on elemental cycling and redox-sensitive contaminant behavior in the vicinity of the RTZ.

Project description:This study investigates the toxicological effects of heavy metals on lithofacies of the subsurface in a drilled hydrocarbon well as well as, to the drilling crew and people in an environment. The pollution levels of selected heavy metals were considered alongside their ecological effects during dry and wet seasons. The health hazard potential of human exposures to the metals, were estimated in terms of intensity and time using the USEPA recommended model. The heavy metal concentration for each layer decreased across the lithofacies as follows; Layer 5> Layer 4> Layer 3> Layer 2> Layer 1. The average concentrations of the heavy metals present in the samples obtained from the formation zone, varied significantly and decreased in the order of Al> Zn> Ni> Pb> Cr> Cu> Cd> As> Hg. The highest concentration of Al, Cu, and Zn in this present study were within the maximum allowable limits whereas, those of As, Cd, Hg and Ni were all above their maximum allowable limits. Among the transition metals analysed, the maximum mean daily dose of Pb (9.18 × 10-6 mg/kg/d) and Cr (1.42 × 10-6 mg/kg/d) were confirmed susceptible to human carcinogens and environmental toxins. The estimated hazard quotient shows that the dermal pathway is the most likely route via which the drilling crew and people in the environment can get contaminated. The cancer risk values for the Pb (7.72 × 10-4), Cd (1.35 × 10-1), Ni (9.97 × 10-3), As (1.50 × 10-1) and Cr (3.16 × 10-3) are all above the acceptable values. The cancer risk contribution for each metal was in the order of As> Cd> Ni> Cr> Pb. Layer 5 had the maximum Geo-accumulation index for the heavy metals considered. This higher Geo-accumulation index noted at the depth in Layer 5 may be attributed to the effect of water basin with turbidity currents, deltas, and shallow marine sediment deposits with storm impacted conditions. Also, the pollution from lead (Pb) in the dry season was maximum with an Igeo value> 5 for all the lithofacies considered because of the low background concentration of the metal. During the wet season, the heavy metal pollution rate was moderate for Zn whereas, it was extremely polluted with respect to Pb. The ecological risk potential of Pb shows that the associated ecological risks range from 536 - 664 in the wet season (i.e. extremely strong) and 2810 - 3480 in dry season (extremely strong). The high level of Pb pollution found in the area at such shallow depth may be due to the sedimentary folds possibly caused by the full spectrum of metamorphic rocks and primary flow structures at shallow depths. This was used to identify the environmental sensitivities of the heavy metals during the dry and wet seasons.

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Conductive catalysis by subsurface transition metals.

Publications

Conductive catalysis by subsurface transition metals.

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