Article 10 - (AQES) Research Group

SEPTEMBER 2015
Also in this issue…
EPA Research Highlights:
The Village Green Project
PM File:
3 Steps to Successful Negotiations
Reactive
Nitrogen
and possible
management
approaches
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Next Month...
Campus Sustainability
Programs:
Walking the Talk
FEATURES
CHAIN REACTION:
A Detailed Look at Reactive
Nitrogen and Possible
Management Approaches
by Christian Hogrefe, U.S. Environmental
Protection Agency Page 4
The six articles in this month’s issue examine various aspects of reactive nitrogen and
potential management approaches, both from a North American and European perspective.
6
24
Impacts of Nitrogen Pollution on
Terrestrial Ecosystems in the United States
by L.H. Pardo, U.S. Department of Agriculture (USDA)
Forest Service; T. Blett, National Park Service; C.M.
Clark, U.S. Environmental Protection Agency; and
L.H. Geiser, USDA Forest Service Page 24
Managing Nitrogen Pollution in the
United States: A Success, a Challenge,
and an Action Plan
Trends in EU Nitrogen Deposition
and Impacts on Ecosystems
by James N. Galloway, University of Virginia; Thomas
L. Theis, University of Illinois at Chicago; and Otto C.
Doering, Purdue University Page 6
Reactive Nitrogen Emissions from
Agricultural Operations
by C. Alan Rotz and April B. Leytem, U.S. Department
of Agriculture’s Agricultural Research Service Page 12
Nitrogen Pollution in the EU: Best
Management Strategies, Regulations,
and Science Needs
by Wilfried Winiwarter, International Institute for Applied
Systems Analysis, Austria; Bruna Grizzetti, European
Commission, Water Resources Unit, Italy; and Mark A.
Sutton, Centre for Ecology & Hydrology, UK Page 18
by Jan Willem Erisman, Louis Bolk Institute and VU
University, the Netherlands; Enrico Dammers, VU
University, the Netherlands; Martin Van Damme, VU
University, the Netherlands and Université Libre de
Bruxellles, Belgium; Nadejda Soudzilovskaia, Louis
Bolk Institute and CML University, the Netherlands;
and Martijn Schaap, TNO, the Netherlands Page 31
Modeling Reactive Nitrogen in North
America: Recent Developments,
Observational Needs, and Future Directions
by Jesse O. Bash, Donna Schwede, Ellen J. Cooter, and
John T. Walker, U.S. Environmental Protection Agency;
Mark W. Shephard, Environment Canada; Karen
E. Cady-Pereira, Atmospheric and Environmental
Research Inc.; Daven K. Henze, University of Colorado;
and Liye Zhu, Colorado State University Page 36
COLUMNS
EPA Research Highlights:
Pollution-Sensing
Benches Provide Local
Air Measurements . . . . 43
by Ann Brown
PM File: Laying the
Groundwork for Successful
Negotiations . . . . . . . . . 44
by David Elam
ASSOCIATION NEWS
Message from the
President: Building
Integrity into the Fabric
of Our Work . . . . . . . . . . 2
by Dallas Baker
Call for Abstracts for
A&WMA’s 109th Annual
Conference & Exhibition,
June 20–23, 2016,
New Orleans, LA . . . . . . 3
IPEP Quarterly:
Mentorship Has Its
Privileges. . . . . . . . . . . . 46
by Diana Kobus
In Memoriam:
Paul J. Lioy . . . . . . . . . . 47
DEPARTMENTS
Advertisers’ Index . . . . . . .
Washington Report . . . . . .
Calendar of Events. . . . . . .
JA&WMA Table of
Contents. . . . . . . . . . . . . . .
45
46
48
48
EM, a publication of the Air & Waste Management Association (ISSN 1088-9981), is published monthly with editorial and executive offices at One Gateway Center, 3rd Floor, 420 Fort Duquesne Blvd., Pittsburgh, PA 15222-1435, USA. ©2015 Air & Waste Management Association. All rights
reserved. Materials may not be reproduced, redistributed, or translated in any form without prior written permission of the Editor. Periodicals postage paid at Pittsburgh and at an additional mailing office. Postmaster: Send address changes to EM, Air & Waste Management Association, One
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Views expressed in editorials are those of the author and do not necessarily represent an official position of the Association.
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Copyright 2015 Air & Waste Management Association
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A&WMA HEADQUARTERS
Stephanie M. Glyptis
Executive Director
Air & Waste Management Association
One Gateway Center, 3rd Floor
420 Fort Duquesne Blvd.
Pittsburgh, PA 15222-1435
1-412-232-3444; 412-232-3450 (fax)
em@awma.org
ADVERTISING
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1-410-584-1993
kprice@networkmediapartners.com
EDITORIAL
Lisa Bucher
Managing Editor
1-412-904-6023
lbucher@awma.org
EDITORIAL ADVISORY COMMITTEE
Mingming Lu, Chair
University of Cincinnati
Term Ends: 2016
John D. Kinsman, Vice Chair
Edison Electric Institute
Term Ends: 2016
John D. Bachmann
Vision Air Consulting
Term Ends: 2016
Gary Bramble, P.E.
AES
Term Ends: 2015
Prakash Doraiswamy, Ph.D.
RTI International
Term Ends: 2017
Ali Farnoud
Trinity Consultants
Term Ends: 2017
Steven P. Frysinger, Ph.D.
James Madison University
Term Ends: 2016
Keith Gaydosh
Affinity Consultants
Term Ends: 2018
C. Arthur Gray, III
CP Kelco-Huber
Term Ends: 2016
Christian Hogrefe
U.S. Environmental Protection Agency
Term Ends: 2016
Ann McIver, QEP
Citizens Energy Group
Term Ends: 2017
Dan L. Mueller, P.E.
Environmental Defense Fund
Term Ends: 2017
Brian Noel
SABIC
Term Ends: 2017
Blair Norris
Ashland Inc.
Term Ends: 2017
Teresa Raine
ERM
Term Ends: 2017
Anthony J. Sadar, CCM
Allegheny County Health Department
Term Ends: 2018
Jacqueline Sibblies
Independent Consultant
Term Ends: 2017
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Building Integrity into
the Fabric of Our Work
by Dallas Baker, P.E., BCEE
president@awma.org
A few years ago, I wrote an article for EM about
an experience that changed my business mindset (see YP Perspective: Five Things I Know Now:
A Professional’s Advice to YPs and Students, EM
August 2001, p. 38). It was a short lesson, but
one that made a lasting impression and one I
think of often. Chance led to my sitting next to
Frank Harrison, CEO of Coca-Cola Consolidated,
at a charity luncheon. As a young leader gaining
more responsibility in my organization and busy
learning the tradecraft of management, I saw an
opportunity to ask him a simple question: “What
are you looking for in a young executive?” Without hesitation he replied, “Integrity, far and away.”
I recall expecting his answer to be more about
skills or credentials, but a man responsible for
leading so many shared his number one qualification in selecting his leaders: integrity.
I find myself in the trust business as an air quality
professional. People are expecting the monitoring
and emissions data, and my characterization of
air quality in my state, to be trustworthy. Good
or bad, people have to believe the information
I present is factual and gathered intentionally to
understand risks to health and welfare. Integrity
is the foundation of building that trust. Lacking
integrity—even a momentary lapse—can undo
years of trust-building efforts of not just me, but
my whole agency, therefore, I can’t afford even
the perception that I’m lacking integrity. Technical
ability and competencies can be developed, and
this is also an area worthy of attention, so that I
can be an effective public official.
A&WMA enjoys a rich history of pioneers working
to advance the field of pollution control. Listening
to Past President Rick Sprott read the accomplishments of those recognized by the Association
during this year’s Honors & Awards Luncheon,
I thought about the integrity of their work. What
became evident, as A&WMA honored its best and
brightest, is that the Association must hold itself
to that standard and weave integrity in the fabric
of all it produces. Just as Mr. Harrison taught me
this important lesson, I encourage you to spend
time investing in the lives of those you influence to
work on professional character, trust, and ethics.
As environmental managers, we must foster trust
in all we do; as leaders in A&WMA, it’s upholding
a legacy set by those of us we remember and
those of us we honor.
This month we prepare for more decisions coming from our regulatory community and the analysis of rulemaking that affects our industry. I am
working diligently to discover more ways to bring
timely, relevant, and trustworthy information to
those who need it, and to position the Association
as the reliable place to go for it. em
Jesse L. Thé
Lakes Environmental Software
Term Ends: 2016
Susan S.G. Wierman
Mid-Atlantic Regional Air
Management Association
Term Ends: 2018
James J. Winebrake, Ph.D.
Rochester Institute of Technology
Term Ends: 2018
2 em september 2015
02_EM0915-Pres-Message.indd 2
Copyright 2015 Air & Waste Management Association
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Agriculture
Figure 1. Sources of new
Nr introduced into the
United States in 2002
(units are Tg N/yr).1
Hab
NF
1
Cul
Managing Nitrogen
Pollution
in the United States
A Success, a Challenge, and an Action Plan
The production of
synthetic fertilizer
through the Haber-Bosch
process, creates manmade reactive nitrogen.
©iStock.com/oticki
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I
n 2002, humans injected 29 teragrams (Tg)
of reactive nitrogen (Nr) into the U.S. environment: agriculture, 19 Tg N; fossil fuel combustion, 5.7 Tg N; industry, 4.2 Tg N.1 This is in
contrast to 6.4 Tg N/yr from the natural source of
Nr—biological nitrogen fixation (BNF) in noncultivated terrestrial ecosystems (see Figure 1).1 This
means that human Nr sources are ~5-fold greater
than natural sources. As noted in the cover story
article, this over-abundance of Nr causes a myriad
of environmental impacts.2-4
Since this analysis was done, two important new
pieces of information have become available—an
update on the magnitude of natural BNF5 and an
estimate of Nr inputs to the United States in 2007.6
Copyright 2015 Air & Waste Management Association
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Na
tu
total, but rather in the sources that contribute
to the total. Specifically, fossil fuel combustion
sources of Nr decreased from 6 to 5 Tg N/yr and
agriculture increased from 23 to 25 Tg N/yr. The
direction of these changes underscores both the
successes and the challenges facing Nr management in the United States.
r
al
BNF
6.4
Haber Bosch
N Fertilizer
Success Story and Challenge
10.9
Stationary
1.9
3.8
Cultivation
BNF
Nonfertilizer
Haber Bosch N
el
7.7
F
o
s
s
i
l Fu
Transportaion
4.2
I nd
us t r
y
On the former, the natural BNF estimate of 6.4
Tg N/yr1 was made in the context that global BNF
in noncultivated systems was on the order of 100
Tg N/yr.7,8 More recently, it has been estimated
that global pre-industrial N fixation was 58 (range:
40–100) Tg N/yr, 5 substantially smaller than the
previous estimate. With this new understanding,
it is probable that natural terrestrial BNF in the
United States is ~3 Tg N/yr (P. Vitousek, personal
communication). This means that humans introduce Nr into the United States at rates that could
be ~10-fold greater than the amount introduced
by natural sources. This underscores the impact
that humans have had on the introduction of Nr to
U.S. systems. The consequences of this added Nr
are very real. It is estimated that the potential health
and environmental damages of anthropogenic N in
the early 2000s in the United States totaled $210
billion/yr (range: $81–$441 billion/yr).9
On the latter, in 2002, anthropogenic Nr sources
totaled 29 Tg N.1 In 2007, they totaled 30 Tg N.6
While the difference between these two is small,
the importance of this comparison is not in the
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The success story is fossil fuel combustion. U.S.
nitrogen oxides (NOx) emissions have decreased
over 2-fold since 1970. They are 5-fold lower than
what they would be without appropriate action. In
addition, NOx emissions are projected to decrease
significantly in the future. This improvement is due
to the marked success of the U.S. Clean Air Act
(and its amendments) and the fact that NOx is a
waste product and comes from point sources (e.g.,
tail pipes, smokestacks). Thus, the NOx is not a
needed resource and it is relatively easy to control.
by James N. Galloway,
Thomas L. Theis, and
Otto C. Doering
James N. Galloway is the
Sidman P. Poole Professor
with the Environmental
Sciences Department at
the University of Virginia,
jng@virginia.edu; Thomas
L. Theis is director of the
Institute for Environmental
Science and Policy at the
University of Illinois at
Chicago, theist@uic.edu;
and Otto C. Doering
is a professor in the
Department of Agricultural
Economics at Purdue
University, doering@
purdue.edu.
The challenge is agriculture. Food cannot be produced without N, and approximately 80% of the N
used in agriculture is lost to the environment along
the food supply chain. Of the estimated 20% of
N that is actually consumed by people, most of
that is lost to the environment due to insufficient
treatment in septic systems and in municipal waste
water treatment plants. So unlike fossil fuel combustion, N has to be used to grow food, and it
is lost to the environment from numerous diffuse
sources along the food supply chain.10
To change this challenge to a success story requires
integrated management strategy along the food
supply chain. This, in turn, requires coordination
among the numerous stakeholders who have the
opportunity to control N losses at specific points in
the food supply chain (see Figure 2).
The major loss points of Nr to the environment are
at either end of the food chain—production and
consumption. For production, the challenge is to
increase N use efficiency of crop and animal production. For consumption, the challenges are to
(1) consume more of the food that is purchased,
(2) consume protein to the U.S. Department
of Agriculture (USDA) dietary guidelines, and
(3) reuse the N in human waste.
Copyright 2015 Air & Waste Management Association
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The Life Cycle of Food
Figure 2 represents various stages in the life cycle
of the food system. The modern food life cycle
involves complex linkages among production, processing, transportation, markets, and acquisition
and consumption with wastage occurring at each
stage. It begins with activities on the field, where
seeds are planted and chemicals, including fertilizer
and pesticides, are applied. Wastage begins almost
at once as water soluble chemicals are drained
from the field during rainfall events, and continues through the production, processing, retailing,
acquisition, preparation, processing, and disposal
life cycle stages. Although some attempts within
each stage are made to recover wasted byproducts,
ultimately from 30% to as much as 50% of food
matter is wasted,11 and as noted above up to 80%
of Nr is discharged to the environment.
What a Waste: Up
to 80% of the N
used to grow food
is discharged to the
environment.
©iStock.com/GgWink
The modern food cycle is driven by consumer
needs and demand. Over time, the human diet
has shifted, from ancient intake based on game,
nuts, and berries (the “Paleolithic” diet) to subsistence agriculture made possible by the advent of
early cultivars of maize, beans, and vegetables, and
to modern agricultural systems with widely varying types of grains, and the proliferation of dairy,
domesticated animals, and processed foods. In all
cases, these “food systems” have been adapted
to, and in turn are driven by, human consumption
preferences and demands. Thus, while present and
past technological and regulatory focuses have
been on waste (which includes soil and nutrients)
associated with on-field production, the habits and
preferences of consumers ultimately determine
environmental and human health impacts. And
yet, little attention has been paid to policies that
can affect consumer decisions on diet and other
food acquisition and handling procedures, and
how these are linked throughout the food cycle,
influencing wastage at all stages.
While the United States, and most developed
countries, have a well-developed agricultural policy, equal effort has not been expended on the
complexities of the food system, and the need
for the development of a health-based food
policy. A first step in that regard is the recently
released draft recommended dietary guidelines
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that take into account the environmental impacts
of food production (see http://www.health.gov/
dietaryguidelines/2015.asp). This is, however, only
a first step. As noted below, what is needed is a
policy that would bring to bear the full economic,
budgetary, regulatory, and taxing functions of the
government; in this case, to bring about a desirable end—reduction of excess Nr in the whole
food system and a healthier population.
Managing Nitrogen Pollution
Control strategies to remove Nr include source
limitation (i.e., reducing the amount of Nr entering
the environment); increased efficiency, which will
lower the requirement for new Nr; and sequestering of existing Nr in the environment. Efforts
to implement these strategies may involve command and control through regulations, other government-based incentives like taxes or subsidies,
voluntary actions, and market-based instruments.
These actions are seldom single approaches and
often involve several actions that are complimentary or reinforcing.12,13
For example, a voluntary approach might be successful because of impending regulations and the
additional incentive of a government subsidy. There
has been great success in the United States reducing Nr in the environment where there were point
sources that came under the U.S. Clean Water Act
and the Clean Air Act. Regulations, government
incentives, market-based instruments, and even
voluntary action all played a role in bringing about
change. The situation is different for agricultural
production and the food chain. Here, the major
challenge for Nr decrease is primarily nonpoint
sources on the production side and something
quite different on the consumption side.1
The opportunities for decreasing the introduction
of Nr to the environment identified in Figure 2
can be broadly classified as those that attempt to
limit Nr from the production side of the system,
and those that might limit Nr on the consumption
side. Success has been mixed in reducing Nr from
agricultural production in the United States. However, advancements have been made in monitoring and validating adaptive N management
designed to reduce Nr applications on working
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Field
Food
Produced
Food
Processed
Food
For Sale
Food
Purchased
Figure 2. Opportunities
for action to decrease N
release to the environment
in the food cycle.
Food
Consumed
N not taken
up by crop
Crop
processing
waste
Food
processing
waste
Food
waste
Food
waste
Human
waste
Improve
NUE
Improve
Recycling
Improve
Recycling
Improve
Recycling
Improve
Recycling
Improve
WWT
(Farmer)
(Farmer)
(Processor)
(Retailer)
Eat to USDA
Guidlines
(Municipality)
(Consumer)
farm fields, while maintaining overall productivity.14 Engineered wetlands have, in some cases,
successfully closed the N-cycle through denitrification and in high-value watersheds denitrification
of wastewater effluents is proactive.1
Still, agriculture has specific exemptions from regulation as compared with point sources under the
Clean Water Act and the Clean Air Act. Programs
to encourage conservation and limit excess nutrients have been largely voluntary since such programs were first developed in the 1930s. These
programs encourage farmer participation through
substantial incentive payments to cover the cost of
actions and sometimes provide additional incentives. The USDA is the primary source of these
funds and programs.
The declaration of impaired waters is the main
regulatory lever for regulating nonpoint excess
nutrients from agriculture. States and other entities are required to identify impaired waters not
meeting the state water quality standards. They
are then required to calculate Total Maximum
Daily Loads (TMDLs), which are the amount of a
pollutant that a water body can receive and still
meet water quality standards for a given water
body. The TMDL implementation plan may
apportion load reductions to nonpoint as well as
point pollution sources.
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The best example of this is the TMDL for the
Chesapeake Bay, which includes the six states
surrounding the Bay as well as the U.S. Environmental Protection Agency (EPA) in the determination and enforcement of nutrient reductions
that include both nonpoint and point sources (see
http://www.epa.gov/chesapeakebaytmdl). Increasingly, environmental groups are pressing for
impaired watershed status and the development
of TMDLs for reductions in excess nutrients, given
that voluntary efforts supplemented by incentives
have not resulted in the level of reductions these
groups desire.
We believe that management to reduce Nr through
changes in the consumption of food products will
become an increasing Nr management focus,
likely starting with the low hanging fruit of waste
reduction. The approach thus far for reducing the
demand for products that require large Nr inputs
and contribute substantial amounts of excess reactive nitrogen have consisted primarily of dietary
guidance, the principle aim of which is proper
nutrition and health (e.g., USDA and World Health
Organization guidelines). Of course, these too are
voluntary in nature. Promulgation of more robust
policies for limiting demand-side Nr would be a
new and different challenge. Policies based solely
on regulatory command and control approaches
are unlikely to be politically or popularly feasible.
Copyright 2015 Air & Waste Management Association
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IT
3
HWC
The annual International Conference on Thermal
Treatment Technologies & Hazardous Waste
Combustors (IT3/HWC) provides a forum for the
discussion of state-of -the-art technical information,
regulations, and public policy on thermal treatment
technologies and their relationship to air emissions,
greenhouse gases, and climate change. Invited and
contributed papers will address approaches to safely
managing waste streams amenable to thermal
treatment processes, and evaluate associated costs,
risks, and impacts.
34th International Conference on
Thermal Treatment Technologies
& Hazardous Waste Combustors
October 20-22, 2015 • Houston, TX
Keynote Plenary Sessions featuring high level executives, including:
Steve Darnell, VP Strategy & Business Improvement at Veolia North America
Scot Shoemaker, Director of Facility Engineering at Clean Harbors
Environmental Services
Bob Patton, Jr., Industrial and Hazardous Waste Permits Section Manager,
Waste Permits Division, Texas Commission on Environmental Quality
Philip J. Schworer, Attorney at Frost Brown Todd LLC
Gary A. Pascoe, PhD, Owner and Principal Scientist, Pascoe Environmental
Consulting
Robert Baxter, President at B3 Systems, Inc.
The question becomes where leverage might
be exerted to inform and/or influence consumer
choices. This might involve the role of subsidies
in the pricing of food, local access to healthy food
alternatives (alleviation of “food deserts and food
insecurity), revision of various taxation policies
(including the imposition of targeted taxation of
certain food and beverage products), facilitation
of food waste recycling, regulatory approaches for
restaurants (e.g., limits on trans fats), and dietary
and nutrition education.15-18 For example, efforts
to change food choices available under the school
lunch program and the Supplemental Nutrition and
Assistance Program (SNAP) in the United States,
which together affect 75 million people, have been
proposed (beneficiaries of SNAP now have almost
complete latitude in the choice of foods).
Many justify restrictions as a means of achieving
better nutrition and improving the health outcomes of the program. In addition, choice restrictions could also operate to limit the choice of food
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classes whose production results in the greatest
level of excess Nr. The dilemma is that freedom
of choice in areas like this is highly prized and
politically difficult to negotiate even within government food programs. Yet, recent studies by the
USDA indicate that education within its food programs can make significant differences. The diets
of children in the Special Supplemental Nutrition
Program for Women, Infants and Children (WIC),
which included a strong educational component,
were more in line with nutritional guidelines than
those of SNAP recipients whose program did not
include such education.19,20
And yet, unlike many production-side programs,
virtually none of the demand-side approaches
outlined above is specifically targeted at reducing
the amount of Nr reaching the environment. It
must be remembered that while Nr is a necessary nutrient, its dietary requirement for humans
is only a little over 4 grams/capita/day out of a total
food need of about 600 grams/capita/day. Thus,
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crafting demand-side policies to control Nr will
almost certainly need to have multiple objectives.
Addressing these issues related to N production
and demand will require cooperation across disciplines, agency missions, and multiple stakeholders.
Spurred by the 2011 recommendations of the EPA
Science Advisory Board,1 scientists and managers
from government, academia, non-government
organizations, and the private sector gathered in
2014 to review science and management related
to reactive nitrogen Nr across EPA, USDA, and
U.S. Geological Survey agencies. The purpose of
the meeting was to develop a research and management partnership among these agencies, in
order to promote sustainable management of Nr.
Workshop participants identified research needs
in monitoring, policy research, technical solutions
research, collaboration, communication, and database alignment. Achieving the common goals of
improving air and water quality, food security, and
human health and welfare will require coordination
of research, policies, and management across agencies and partnerships with the private sector.21,22
Summary
Anthropogenic activities in the United States inject
up to 10-fold more Nr into the environment than
do natural terrestrial processes. This imbalance has
significant negative impacts on both environmental and human health. Significant success has been
achieved in the decrease of NOx emissions from
fossil fuel combustion. Equivalent successes are
needed in the area of food production, but there
are significant challenges at both the food production and consumption portions of the food supply
chain. Ultimate success will only come when the
entire system is optimized to produce food with the
minimum of environmental cost. For this to occur,
all stakeholders must be seated at the table! em
References
1. EPA. Reactive Nitrogen in the United States; An analysis of inputs, flows, consequences, and management options; U.S. Environmental Protection Agency, Washington, DC, 2011.
2. Hogrefe, C. Chain Reaction: A detailed look at reactive nitrogen and possible management approaches; EM September 2015, 4.
3. Pardo, L.H.; Blett, T.; Clark, C.M.; Geiser, L.H. Impacts of Nitrogen Pollution on Terrestrial Ecosystems in the United States; EM September
2015, 24.
4. Erisman, J.W.; Dammers, E.; Van Damme, M.; Soudzilovskaia, N.; Schaap M. Trends in EU Nitrogen Deposition and Impacts on Ecosystems;
EM September 2015, 31.
5. Vitousek, P.M.; Menge, D.N.L.; Reed, S.C.; Cleveland, C.C. Biological Nitrogen Fixation: Rates, patterns, and ecological controls in terrestrial
ecosystems; Phil. Trans. R. Soc. B 2013, 368, 20130119.
6. Houlton, B.Z.; Boyer, E.; Finzi, A.; Galloway, J.; Leach, A.; Liptzin, D.; Mellilo, J.; Rosenstock, T.S.; Sobota, D.; Townsend, A.R. Intentional versus
Unintentional Nitrogen Use in the United States: Trends, efficiency, and implications; Biogeochemistry 2013, 114, 11-23.
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A.; Wasson, M.F. Global Patterns of Terrestrial Biological Nitrogen (N2) Fixation in Natural Ecosystems; Global Biogeochem. Cycles 1999,
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