Streamlining Rich Media Communications In A Non-Profit organization: Making Meetings Meaningful

This study is an organizational diagnosis of a highly centralized non-profit organization, which desired to reduce the number of monthly committee meetings. Using an emergent design flexibility strategy. the findings revealed that because the members of the organization were accustomed to receiving frequent rich media communication, they may resist a reduction in meetings. Therefore, the study offers four recommendations to reduce the number of meetings to increase member satisfaction. Because of contradictory findings compared to existing research, two areas within the study of leadership are offered further research

Exploring The Role of Spirituality Within Intense Interpersonal Conflicts

The foundation for determining the approach to manage interpersonal conflict extends across two poles of consideration: the concern for self and the concern for others. This assumption has influenced the calculated response people would exhibit when experiencing an intense interpersonal conflict. However, recent findings within the realm of spirituality challenge these foundational assumptions. Spirituality literature contends that individuals may place substantial emphasis upon transcendent concerns rather than temporal concerns such as self and others. This study explores whether spirituality plays a role in the conflict management process through a phenomenological research investigation. The researcher interviewed 10 participants, who served as faculty members in the philosophy and religion department at a college in the Midwest. The results of the data analysis suggest that spirituality serves a crucial role in the conflict management process. When a stimulus violates the spirituality of an individual, an intense interpersonal conflict may erupt. This study offers a structural model of the conflict management process and implications of the role spirituality serves within the management of interpersonal conflicts for managers and leaders

An Fe-N_2 Complex That Generates Hydrazine and Ammonia via Fe═NNH_2: Demonstrating a Hybrid Distal-to-Alternating Pathway for N_2 Reduction

Biological N_2 fixation to NH_3 may proceed at one or more Fe sites in the active-site cofactors of nitrogenases. Modeling individual e–/H+ transfer steps of iron-ligated N_2 in well-defined synthetic systems is hence of much interest but remains a significant challenge. While iron complexes have been recently discovered that catalyze the formation of NH_3 from N_2, mechanistic details remain uncertain. Herein, we report the synthesis and isolation of a diamagnetic, 5-coordinate Fe═NNH_2+ species supported by a tris(phosphino)silyl ligand via the direct protonation of a terminally bound Fe-N_2– complex. The Fe═NNH_2+ complex is redox-active, and low-temperature spectroscopic data and DFT calculations evidence an accumulation of significant radical character on the hydrazido ligand upon one-electron reduction to S = 1/2 Fe═NNH_2. At warmer temperatures, Fe═NNH_2 rapidly converts to an iron hydrazine complex, Fe-NH_2NH_2+, via the additional transfer of proton and electron equivalents in solution. Fe-NH_2NH_2+ can liberate NH_3, and the sequence of reactions described here hence demonstrates that an iron site can shuttle from a distal intermediate (Fe═NNH_2+) to an alternating intermediate (Fe-NH_2NH_2+) en route to NH_3 liberation from N_2. It is interesting to consider the possibility that similar hybrid distal/alternating crossover mechanisms for N_2 reduction may be operative in biological N_2 fixation

A 10^6‑Fold Enhancement in N_2‑Binding Affinity of an Fe_2(μ-H)_2 Core upon Reduction to a Mixed-Valence Fe^(II)Fe^I State

Transient hydride ligands bridging two or more iron centers purportedly accumulate on the iron–molybdenum cofactor (FeMoco) of nitrogenase, and their role in the reduction of N_2 to NH_3 is unknown. One role of these ligands may be to facilitate N_2 coordination at an iron site of FeMoco. Herein, we consider this hypothesis and describe the preparation of a series of diiron complexes supported by two bridging hydride ligands. These compounds bind either one or two molecules of N_2 depending on the redox state of the Fe_2(μ-H)_2 unit. An unusual example of a mixed-valent Fe^(II)(μ-H)^2Fe^I is described that displays a 10^6-fold enhancement of N_2 binding affinity over its oxidized congener, quantified by spectroscopic and electrochemical techniques. Furthermore, these compounds show promise as functional models of nitrogenase as substantial amounts of NH_3 are produced upon exposure to proton and electron equivalents. The Fe(μ-H)Fe(N2_) sub-structure featured herein was previously unknown. This subunit may be relevant to consider in nitrogenases during turnover

Catalytic conversion of nitrogen to ammonia by an iron model complex

The reduction of nitrogen (N_2) to ammonia (NH_3) is a requisite transformation for life. Although it is widely appreciated that the iron-rich cofactors of nitrogenase enzymes facilitate this transformation, how they do so remains poorly understood. A central element of debate has been the exact site or sites of N_2 coordination and reduction. In synthetic inorganic chemistry, an early emphasis was placed on molybdenum because it was thought to be an essential element of nitrogenases and because it had been established that well-defined molybdenum model complexes could mediate the stoichiometric conversion of N_2 to NH_3 (ref. 9). This chemical transformation can be performed in a catalytic fashion by two well-defined molecular systems that feature molybdenum centres. However, it is now thought that iron is the only transition metal essential to all nitrogenases, and recent biochemical and spectroscopic data have implicated iron instead of molybdenum as the site of N_2 binding in the FeMo-cofactor. Here we describe a tris(phosphine)borane-supported iron complex that catalyses the reduction of N_2 to NH_3 under mild conditions, and in which more than 40 per cent of the proton and reducing equivalents are delivered to N_2. Our results indicate that a single iron site may be capable of stabilizing the various N_xH_y intermediates generated during catalytic NH_3 formation. Geometric tunability at iron imparted by a flexible iron–boron interaction in our model system seems to be important for efficient catalysis. We propose that the interstitial carbon atom recently assigned in the nitrogenase cofactor may have a similar role, perhaps by enabling a single iron site to mediate the enzymatic catalysis through a flexible iron–carbon interaction

Fe–N_2/CO complexes that model a possible role for the interstitial C atom of FeMo-cofactor (FeMoco)

We report here a series of four- and five-coordinate Fe model complexes that feature an axial tri(silyl)methyl ligand positioned trans to a substrate-binding site. This arrangement is used to crudely model a single-belt Fe site of the FeMo-cofactor that might bind N_2 at a position trans to the interstitial C atom. Reduction of a trigonal pyramidal Fe(I) complex leads to uptake of N_2 and subsequent functionalization furnishes an open-shell Fe–diazenido complex. A related series of five-coordinate Fe–CO complexes stable across three redox states is also described. Spectroscopic, crystallographic, and Density Functional Theory (DFT) studies of these complexes suggest that a decrease in the covalency of the Fe–C_alkyl interaction occurs upon reduction and substrate binding. This leads to unusually long Fe–C_alkyl bond distances that reflect an ionic Fe–C bond. The data presented are contextualized in support of a hypothesis wherein modulation of a belt Fe–C interaction in the FeMo-cofactor facilitates substrate binding and reduction

Proton-Coupled Reduction of an Iron Cyanide Complex to Methane and Ammonia

Nitrogenase enzymes mediate the six-electron reductive cleavage of cyanide to CH_4 and NH_3. Herein we demonstrate for the first time the liberation of CH_4 and NH_3 from a well-defined iron cyanide coordination complex, [SiP^(iPr)_3]Fe(CN) (where [SiP^(iPr)_3] represents a tris(phosphine)silyl ligand), on exposure to proton and electron equivalents. [SiP^(iPr)_3]Fe(CN) additionally serves as a useful entry point to rare examples of terminally-bound Fe(CNH) and Fe(CNH_2) species that, in accord with preliminary mechanistic studies, are plausible intermediates of the cyanide reductive protonation to generate CH_4 and NH_3. Comparative studies with a related [SiP^(iPr)_3]Fe(CNMe_2) complex suggests the possibility of multiple, competing mechanisms for cyanide activation and reduction

Characterization of an Fe≡N−NH_2 Intermediate Relevant to Catalytic N_2 Reduction to NH_3

The ability of certain transition metals to mediate the reduction of N_2 to NH_3 has attracted broad interest in the biological and inorganic chemistry communities. Early transition metals such as Mo and W readily bind N_2 and mediate its protonation at one or more N atoms to furnish M(N_xH_y) species that can be characterized and, in turn, extrude NH_3. By contrast, the direct protonation of Fe–N_2 species to Fe(N_xH_y) products that can be characterized has been elusive. Herein, we show that addition of acid at low temperature to [(TPB)Fe(N_2)][Na(12-crown-4)] results in a new S = 1/2 Fe species. EPR, ENDOR, Mössbauer, and EXAFS analysis, coupled with a DFT study, unequivocally assign this new species as [(TPB)Fe≡N–NH_2]^+, a doubly protonated hydrazido(2−) complex featuring an Fe-to-N triple bond. This unstable species offers strong evidence that the first steps in Fe-mediated nitrogen reduction by [(TPB)Fe(N_2)][Na(12-crown-4)] can proceed along a distal or “Chatt-type” pathway. A brief discussion of whether subsequent catalytic steps may involve early or late stage cleavage of the N–N bond, as would be found in limiting distal or alternating mechanisms, respectively, is also provided

Sobre as origens e o desenvolvimento do Estado moderno no Ocidente

São Paulo - SPRevista Lua NovaNo 1

A computational study of the heterogeneous synthesis of hydrazine on Co3Mo3N

Periodic and molecular density functional theory calculations have been applied to elucidate the associative mechanism for hydrazine and ammonia synthesis in the gas phase and hydrazine formation on Co3Mo3N. We find that there are two activation barriers for the associative gas phase mechanism with barriers of 730 and 658 kJ/mol, corresponding to a hydrogenation step from N2 to NNH2 and H2NNH2 to H3NNH3, respectively. The second step of the mechanism is barrierless and an important intermediate, NNH2, can also readily form on Co3Mo3N surfaces via the Eley–Rideal chemisorption of H2 on a pre-adsorbed N2 at nitrogen vacancies. Based on this intermediate a new heterogeneous mechanism for hydrazine synthesis is studied. The highest relative barrier for this heterogeneous catalysed process is 213 kJ/mol for Co3Mo3N containing nitrogen vacancies, clearly pointing towards a low-energy process for the synthesis of hydrazine via a heterogeneous catalysis route